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Inflammatory bowel disease (IBD) involves oxidative stress, chronic inflammation, and gut microbiota dysbiosis, complicating therapeutic intervention. Herein, we engineer a robust living therapeutic platform via a biomimetic nanoarmoring strategy. A uniform FDA-approved calcium carbonate (CaCO3) nanocoating is in situ mineralized on the surface of the probiotic Escherichia coli Nissle 1917 (EcN) preassembled with the flavonoid luteolin (Lut), creating the nanocomposite EcN-Lut/CaCO3. This nanoarmoring strategy enhances bacterial viability under simulated gastrointestinal conditions (a 100-fold survival increase) and enables colon-specific delivery. The composite demonstrates potent reactive oxygen species scavenging (∼100%) and immunomodulatory capacity in vitro, downregulating pro-inflammatory cytokines (TNF-α, IL-6, IL-1β, IL-17A) while elevating anti-inflammatory IL-10. In a DSS-induced murine colitis model, EcN-Lut/CaCO3 significantly attenuated disease severity, restoring colon length (a 57.30% recovery compared to healthy control), reducing the disease activity index by 72.73% relative to the DSS group, and improving histopathology. Transcriptomic analysis reveals dual regulation of host signaling pathways with activation of cAMP/cGMP-PKG metabolic cascades and suppression of IL-17/TNF inflammatory pathways. Concurrently, 16S rRNA sequencing shows that the nanoarmored platform effectively reverses dysbiosis, selectively enriching beneficial genera such as Lactobacillus and Muribaculaceae while suppressing proteobacterial pathobionts. This work presents a generalizable nanoarmoring strategy that transforms fragile probiotics into intelligent, multifunctional living therapeutics, offering a powerful approach for the targeted treatment of IBD and other complex inflammatory disorders.

Nanofluidic ionic transistors typically require gate voltages above 1 V and operate only at submillimolar ionic strengths, limiting their biocompatible applications. We demonstrate ionic transistors consisting of single sub-10 nm nanopores drilled in van der Waals (vdW) heterostructures with internal gate electrodes made of few-layer graphene. These devices deliver up to 10-fold current modulation at gate voltages as low as 0.3 V in 10 mM KCl, and ∼2-fold modulation at near-physiological 100 mM KCl. Baseline conductance with no gate shows surface-charge-dominated transport below 100 mM KCl, consistent with negatively charged hBN walls and ∼5 nm opening of the pores. The surface charge and the electrochemical asymmetry introduced by the three-electrode configuration govern the device's behavior: negative gate voltage (VG) enriches ionic concentrations and enhances current, whereas positive VG induces a local depletion zone that suppresses transport. The current modulation by VG is dependent on the polarity of the transmembrane potential and leads to ion current rectification. Molecular dynamics simulations of a nanopore in a hBN-graphene-hBN stack reveal confinement and surface charge-dependent suppression of the relative permittivity of interfacial water. Continuum modeling with radially varying interfacial water permittivity reproduces the asymmetric I-V characteristics and explains how the embedded gate sculpts local potential and ion concentrations. By enabling sub-0.5 V control of ionic transport at up to 100 mM salt concentrations, these devices address a key need in nanofluidics to create low-power ionic circuits and biosensing.

Rapid and multiplexed detection of urinary microRNAs (miRNAs) is crucial for the noninvasive diagnosis and monitoring of bladder cancer. In this study, we develop a dual-channel fluorescence platform based on filler-mediated quantum dot-DNA nanospheres for simultaneous detection of miRNA-21 and miRNA-96. The nanospheres are constructed via a streptavidin-biotin cross-linked bidirectional hybridization chain reaction and compacted by phenyl-lactic acid, enabling high-density encapsulation of distinct QDs. Upon target miRNA recognition, a strand-displacement cascade triggers nanosphere disassembly and QDs release, restoring well-resolved fluorescence at 500 and 624 nm. This enzyme-free, extraction-free assay is completed in 40 min. It achieves attomolar-level sensitivity, with detection limits of 30 aM for miRNA-21 and 40 aM for miRNA-96, while maintaining high selectivity against mismatched and nontarget miRNAs. Clinical validation using urine samples from 45 patients with bladder cancer, 22 patients with other urological diseases, and 20 healthy controls indicated strong concordance with quantitative polymerase chain reaction. Integrated dual-miRNA analysis significantly enhanced diagnostic performance, yielding 91.0% sensitivity, 80.0% specificity, and an area under the curve of 0.91. The platform provides a rapid tool for noninvasive miRNA profiling, with potential to distinguish bladder cancer from healthy individuals and other urological diseases, thereby improving bladder-cancer screening, stratification, and recurrence monitoring.

Efficient nanoparticle migration to sentinel lymph nodes (SLNs) is vital for immunotherapy and diagnostics, yet the governing mechanisms remain controversial. Current paradigms assume a 100 nm size cutoff, where larger nanoparticles rely exclusively on slow, cell-mediated transport rather than rapid noncell-mediated migration, including diffusion and convection. Here, we reveal a predominant noncell-mediated delivery mechanism using 120 nm gold particles as a model. We adopt a multiscale correlative imaging approach, integrating Raman imaging, optical microscopy, and electron microscopy, to quantify in vivo transport pathways. Unexpectedly, the noncell-mediated pathway accounts for approximately 82% of nanoparticle migration to the SLN, while cell-mediated delivery contributes only 18%. Upon entry into the SLNs, particles are rapidly internalized by resident macrophages for prolonged retention. This work helps to refine the fundamental framework of lymphatic trafficking, providing insights into the design of vaccines and lymph node-targeted therapeutics.

Ag nanodendrites (AgNDs) were directly grown on nonanodized metallic Ti via potentiostatic electrodeposition (PED) to produce a simple and controllable SERS substrate. The effects of electrolyte composition and hydrodynamic conditions on dendritic growth were systematically investigated, revealing that the combined presence of a supporting electrolyte (NaNO3) and magnetic stirring enables sustained tip-driven growth and hierarchical branching. An optimal dendritic architecture was obtained at 2.0 V for 60 s, yielding the highest SERS enhancement. The strongest responses were found to arise from an experimentally optimal morphological regime characterized by intermediate surface coverage (∼50-65%) and well-developed secondary branching, which maximizes hotspot density while preserving interbranch gaps. Postdeposition conditioning proved critical, as mild PBS conditioning (50 mM) effectively suppressed intrinsic background signals while preserving dendritic morphology and establishing a chemically compatible interface for subsequent molecular and biomolecular interactions. The optimized AgND/Ti substrate exhibited robust analytical performance, achieving a limit of detection (LoD) of 3 × 10-8 M for Rhodamine 6G and consistent enhancement across chemically distinct dyes, including methylene blue and crystal violet. Beyond small-molecule detection, the substrate demonstrated compatibility with biomolecular SERS measurements and controlled surface functionalization. Biomolecular species produced reproducible amide-dominated spectral features, while MPA-EDC/NHS chemistry enabled stable covalent immobilization of monoclonal anti-α-fetoprotein antibodies (Ab-AFP) while maintaining a detectable and reproducible SERS response under the applied experimental conditions. Overall, these results establish clear morphology-performance and surface-functionality relationships in AgND/Ti substrates and highlight their potential as integrated platforms for molecular and biomolecular SERS-based detection.

The creation of colloidal allotropes, structures with identical composition but divergent architectures and properties, represents a key aspect for controlled material fabrication yet it is highly challenging. Particularly, a general and efficient method for fabricating such nanoallotropes over large areas remains elusive. Here, we report a direct magnetic assembly strategy to construct nanoallotropes via controlling the Fe3O4@SiO2 nanoellipsoid orientation during drying. By tuning the magnetic field direction, the electrostatic and magnetic dipolar interactions, along with a physical boundary, drive the formation of amorphous photonic glasses, hexagonal close-packed (hcp) crystals, as well as multiple monoclinic crystals whose lattice parameters are continuously tunable. Capitalizing on this tunability, we develop a revolutionary photonic ink (P-ink) that enables single-ink, multicolor writing and printing. This all-inorganic ink is fully recyclable and produces high-resolution, nonfading, and glare-free colors on virtually any substrate. This work not only provides insights into the controlled assembly of anisotropic colloids but also establishes a versatile platform for applications in anticounterfeiting, color printing, and functional photonic devices.

We report a complete neutron-scattering and molecular dynamics investigation of the structure and dynamics of monomer and polymer phases of C60 carbon peapods. Above ∼250 K, the physics of the confined chains can fully be described without accounting for the nanotube, the latter merely playing the role of a container for a 1D system─the system can be described as an unpinned state in the extended Frenkel-Kontorova framework. As the temperature is lowered below about 250 K, we observe a progressive damping of the longitudinal acoustic phonons, measured in both monomer and polymer data. As a set of experimental observations suggest that this damping can be attributed neither to a 3D ordering of the chains nor to a transition driven by rotation-rotation-translation coupling, we attribute it to an increase in the chain-nanotube interaction. This translates into a progressive pinning of the C60 chains on the nanotube lattice as the temperature is lowered and explains the observed low-temperature damping.

Macrophages play a critical role in the development of the tumor microenvironment (TME). Recruited macrophages in the TME differentiate into various phenotypes, each with a distinct profile of secreted cytokines. To describe and understand this large heterogeneity, we developed nested nanowell arrays for the multiplexed analysis of secreted proteins at the single cell level. The array consists of more than 100,000 wells on a cyclic olefin copolymer (COC) substrate. Each well contains seven smaller indents for cocapturing functionalized beads and can be operated with standard laboratory equipment such as pipettes and microscopes. The barcoded beads capture cytokines of interest and allow their quantification via sandwich immunoassays. We developed an image analysis tool and quantified 10 proteins secreted from single macrophages and investigated the effects of stimulation and drug treatment. We found that interleukin (IL)-1β, IL-8, and macrophage inflammatory protein 1α (MIP-1α) were highly secreted by more than 43% of the macrophages, with an increase of MIP-1α secretion under treatment with the chemotherapeutic drugs paclitaxel or docetaxel. Pairwise protein analysis confirmed cosecretion of IL-1β and IL-6 in macrophages stimulated with IL-4/IL-13, which were identified as part of a critical pathway in multiple myeloma before. We also demonstrate further multiplexing with three and four cosecreted proteins, together with assessing the cell viability as an additional parameter important for drug testing. In summary, we have shown that our nested nanowell arrays are an easy-to-use analytical tool for basic research, and we believe that it can be employed for diagnostics and personalized medicine, e.g., for investigation of cancer and immune cells from a biopsy or circulating tumor cells obtained from a liquid biopsy.

Airborne nanoplastic (NP) pollution is an emerging threat to respiratory health. Although inhaled NPs rapidly acquire a protein corona that shapes their bioactivity, the consequences of this process in cancer-susceptible lungs remain unclear. Here, we investigated whether NPs form a disease-specific pathogenic protein corona in lung adenocarcinoma that rewires immune signaling and accelerates tumor progression. Polyethylene terephthalate (PET) NPs were generated by mechanical fragmentation and extensively characterized. In tumor-bearing mice, inhaled PET NPs accelerated tumor growth relative to controls. Proteomic analysis of PET NPs incubated with bronchoalveolar lavage fluid from patients with lung adenocarcinoma identified lysozyme (LYZ) as a selectively enriched corona component associated with tumor stage and metastasis. Corona formation induced conformational remodeling of LYZ, enhanced its enzymatic activity, and prolonged its membrane retention. Mechanistically, corona-bound LYZ engaged Toll-like receptor 4 and activated a PGRN-LXRα signaling axis, thereby increasing lysosomal acidification-dependent efferocytosis, promoting M2 macrophage polarization, and reducing CD8+ T-cell infiltration. In vivo, AAV9-mediated knockdown of LYZ or PGRN attenuated PET NP-induced efferocytosis, reversed immunosuppressive reprogramming, restored CD8+ T-cell infiltration, and suppressed tumor growth, demonstrating the functional requirement for this corona pathway. These findings establish disease-derived PET NP coronas as active nano-bio interfaces that connect environmental PET NP exposure with efferocytosis-driven immune evasion in lung adenocarcinoma. This work provides a mechanistic link between airborne NPs and tumor progression in susceptible hosts and highlights corona-mediated signaling as a potential therapeutic target and environmental health concern.

In this study, the development of boron-doped zinc oxide nanorods (B-ZnO NRs) as an innovative photocatalyst for the degradation of organic pollutants under UV-A light was investigated. ZnO NRs, doped with varying concentrations of boron, were synthesized via a hydrothermal method, and their structural, optical, electrical, and photocatalytic properties were systematically characterized. The photocatalytic performance of B-ZnO NRs was evaluated under varying pH conditions, contaminant concentrations, and reaction times, while their electrical properties were analyzed by examining the conduction mechanism using the Arrhenius and Mott variable range hopping (VRH) conduction models. Results indicated that boron doping altered the conduction mechanism of ZnO as predicted by these models. In addition, boron doping enhanced electrical conductivity, with DC conductivity increasing up to 5-fold and alternating current conductivity by 3-fold compared to undoped ZnO. A significant enhancement in photocatalytic efficiency was observed, with B-ZnO exhibiting up to 140% higher degradation efficiency at pH 10 compared to pure ZnO. In addition, a Taguchi statistical optimization approach was employed to identify the most influential parameters affecting photocatalytic performance, including pH, reaction time, contaminant concentration, and boron doping levels. Optimal conditions were determined to be pH 10, a contaminant concentration of 2 μM, a reaction time of 90 min, and a boron doping level of 7%. Boron doping significantly improved the photocatalytic activity of ZnO nanorods, making them a promising candidate for advanced water treatment, hydrogen production, and environmental sensing applications.

We report the formulation and printing of Cu inks composed of binary mixtures of colloidal ∼5 nm Cu nanocrystals (NCs) and ∼500 nm Cu microcrystals (MCs) and postdeposition chemical and low-temperature thermal treatments to achieve micron-thick, high-conductivity metal traces that yield high-performance, printed radio frequency (RF) electronic devices. Solid-state NH4Cl treatment of binary Cu NC/MC mixed films removes insulating ligands and surface oxides and establishes Cl--mediated surface chemistry that drives NC-enabled "nano-soldering" between MCs and increased MC faceting and interparticle necking. Subsequent mild annealing under N2 promotes further densification to yield micron-scale films with resistivities as low as ∼14.5 times that of bulk Cu for optimized 75 wt % NC/MC films after annealing at 150 °C for 5 min. By formulating these binary NC/MC systems in α-terpineol/ethyl cellulose/poly(vinylpyrrolidone) vehicles, we obtain non-Newtonian inks compatible with both screen printing and direct ink writing (DIW) and we deposit micron-thick patterned conductive traces on flexible substrates. Screen-printed, flexible RF inductively coupled interdigitated capacitors are fabricated from the mixed NC/MC inks and achieve Q = 4.89, corresponding to ∼68% of a bulk-Cu reference. DIW produces over 100 μm thick CAD-defined traces with an average resistivity of 95 ± 22.6 μΩ·cm. We show that NC-enabled processing of mixed NC/MC systems yield manufacturable, high-frequency metal components for printed Internet of Things platforms.

Psoriasis is a chronic autoimmune skin disorder primarily driven by dendritic cells (DCs). However, the full therapeutic potential of antipsoriatic agents like calcipotriol (Cal) hinges on the precise and efficient delivery to DCs. Herein, a nanovehicle fabricated using keratinocyte-derived apoptotic vesicles (apoEVs) is proposed to enhance drug accumulation in DCs and synergistically modulate DC function. Specifically, the phosphatidylserine exposed on the apoEV surface serves as an "eat-me" signal, facilitating specific recognition and engulfment by DCs. This process mimics the natural efferocytic clearance of apoptotic keratinocytes by DCs in the skin. Moreover, apoEVs intrinsically inhibit DC maturation by eliciting efferocytosis-mediated immunosuppressive signals. To enable transdermal administration, Cal-loaded apoEVs were integrated into dissolvable microneedles (MNs). As a consequence, the Cal-apoEV MNs demonstrated superior capability in reprogramming DCs from a pro-inflammatory to a tolerogenic phenotype, thereby suppressing the pathogenic inflammatory loop and ameliorating psoriatic symptoms. Notably, Cal-apoEV MNs remodeled the psoriatic immune microenvironment toward a tolerogenic state, characterized by enhanced regulatory T cell infiltration. The present study reveals that the keratinocyte-derived nanovehicles can not only enhance the accumulation of Cal in DCs but also synergistically reprogram DCs, providing a promising strategy for treating immune-mediated skin diseases.

Messenger RNA (mRNA) lipid nanoparticles (mRNA-LNPs) are central to emerging vaccines and therapeutics, but their wide implementation is constrained by limited endosomal escape and instability during long-term storage and freezing. While buffers are routinely optimized to prevent instability, the impact of buffer on the internal structural organization of LNPs and, consequently, their delivery efficiency remain unresolved. Here, we study the impact of storage in Tris, histidine, and citrate buffers for mRNA-LNPs formulated with LP-01, MC3, and SM-102 ionizable lipids. We demonstrate that storage buffer identity and concentration govern mRNA-LNP internal ordering before and after freeze-thaw and are thus critical parameters for engineering high-performance formulations. Deconvoluting ordered phases into an mRNA-lipid region and excess lipid region reveals the importance of excess ionizable lipid behavior in enhancing endosomal escape. Prior to freezing, citrate buffer enhances transfection efficiency by promoting a transition to the fusogenic inverse hexagonal (HII) phase earlier during acidification, facilitated by a greater amount of ordered excess ionizable lipid. In contrast, Tris buffer provides the highest transfection efficiency after freeze-thaw by preventing aggregation and cargo loss while promoting favorable internal structure. Increasing Tris concentration from 10 to 50-150 mM leads to mRNA-rich bleb formation in freeze-thawed mRNA-LNPs, which improves freeze-thaw stability and thus transfection efficiency by mitigating mRNA-lipid adduct formation and accommodating a larger excess ionizable lipid region to facilitate HII phase formation. These findings establish a direct structural link between buffer conditions, particle size, internal morphology, and transfection efficiency, highlighting the importance of buffer composition in modulating mRNA-LNP performance.

Carbon nanotubes (CNTs), combining excellent electrical and optoelectronic properties with low-temperature processability, provide a compelling materials platform for monolithic three-dimensional (M3D) integration that unifies digital logic in complementary field-effect transistor (CFET) architecture and functional sensing elements with three-dimensionally structured nondigital functional blocks. However, such a fully integrated system has not yet been experimentally demonstrated. Here, we report CNT-based digital circuits implemented in a true CFET architecture, in which vertically stacked P- and N-FETs share an identical footprint and exhibit well-balanced performance through structural engineering. A full suite of logic functions, including inverters, NOR, OR, NAND, AND gates, as well as a 4-transistor static random-access memory cell and a five-stage ring oscillator are successfully demonstrated. The CFET inverters exhibit rail-to-rail operation with large noise margins and a peak voltage gain of 147 at a supply voltage of 1 V, while maintaining a gain of 9.7 with only 3.3 pW static power consumption at 0.2 V. In parallel, CNT photodiodes are vertically stacked and cascaded to form a 3D optical sensor that delivers nearly twice the photovoltage of planar counterparts. By monolithically integrating the 3D CNT photodiode with a CNT-based CFET inverter, we further demonstrated a prototype "sensing-and-computing" module in which optical power and spectral information are directly sensed and processed within a single monolithic CNT-based block. This work establishes CNTs as a unified platform for high-density, low-power M3D integration toward near-/in-sensor and edge-computing applications.

Optically active spin-based solids are vital for spintronics, yet materials with robust, room-temperature spin polarization remain elusive. Eu2+ ions, with their high-spin S = 7/2 ground state, are ideal candidates, but their emission spin polarization is typically quenched at elevated temperatures, as thermal fluctuations easily overwhelm the finite Zeeman splitting energy. Here, we demonstrate high-efficiency, room-temperature spin-polarized luminescence from trace-doped CsCaCl3:Eu2+ perovskite nanocrystals, stabilized via in situ glass crystallization. The system exhibits a high degree of circular polarization of ≈45% at cryogenic temperatures, arising from the spin-coupled 4f65d1 state. We further elucidated the underlying magnetic interactions, revealing a concentration-driven crossover from ferromagnetic to antiferromagnetic coupling, definitively confirmed by the sign reversal of the Weiss constant. Crucially, the strong exchange interaction intrinsic to this specific spin-bound configuration functions as a locking mechanism that preserves the Zeeman splitting against thermal fluctuations, enabling distinct circularly polarized emission even at room temperature. We leverage this to demonstrate reversible, room-temperature emission magnetic encoding, identifying Eu2+-doped perovskites as a platform for ambient-condition spintronic and quantum technologies.

The design of a cost-effective, sustainable bifunctional electrocatalyst from earth-abundant materials for the advancement of water splitting is urgently needed. Herein, we report an interphase-engineered Fe-doped α-Mo15Se19/CoSeO3 nanosheet array on carbon fabric (CF) through an in situ oxidation-selenization strategy, employed as a self-supported bifunctional electrode for overall water splitting. Quantitative X-ray photoelectron spectroscopy (XPS) analysis reveals that Fe incorporation induces distinct electronic modulation and interfacial charge redistribution. This bidirectional electronic interaction optimizes the adsorption energetics of reaction intermediates and significantly promotes charge-transfer kinetics. Consequently, the optimized heterostructure exhibits exceptional bifunctional activity, requiring overpotentials of only 207 mV at 20 mA cm-2 for the oxygen evolution reaction (OER) and 98 mV at 10 mA cm-2 for the hydrogen evolution reaction (HER). When integrated into an alkaline water electrolyzer, the system delivers a benchmark cell voltage of 1.52 V at 10 mA cm-2 and maintains stable operation for 100 h at 50 mA cm-2 with a minor voltage increase of only 9.6%. The results show that interfacial engineering and electronic modulation are effective tools for regulating catalytic activity and stability. This work offers a viable foundation for developing high-performance, noble-metal-free bifunctional electrocatalysts for alkaline water splitting.

Recently, targeted protein degradation (TPD) strategies have emerged as an effective tool for addressing undruggable targets in both biomedical research and the pharmaceutical industry, selectively binding proteins of interest and targeting them to the intracellular degradation machinery for degradation. However, the targeting of extracellular proteins with current degradation tools requires a tedious, case-specific selection and design process based on lysosomal trafficking of cell surface receptors. Here, we introduce Macropinocytosis-Targeting Chimeras (MapTACs), a TPD platform that exploits macropinocytosis, a receptor-independent endocytic process, to deliver extracellular proteins to lysosomes for degradation. Using dextran as a versatile scaffold conjugated to protein-binding aptamers or antibodies, we demonstrate that MapTACs efficiently degrade monocyte chemotactic protein-1 (MCP-1) in a time-, dose-, and macropinocytosis-dependent manner. Importantly, without the need for receptor-specific modifications, MapTACs exhibit broad applicability to a variety of cell types and extracellular protein targets (MCP-1, tumor necrosis factor-α, and interferon-γ). In vivo, TNF-α-targeting MapTACs effectively and specifically reduce the levels of TNF-α in an LPS-induced acute inflammation model, attenuating lung injury, with a half-life of approximately 0.72 h and predominant accumulation in the liver and lung, where F4/80-positive monocytes/macrophages serve as the primary uptake cells. By overcoming the limitations of the receptor-based TPD strategy, MapTAC provides a universal, cost-effective, and scalable platform for extracellular protein degradation, facilitating the development of targeted protein degradation tools and opening opportunities for therapeutic intervention in cancer, inflammation, and other diseases.

The rational regulation of the surface reconstruction in transition-metal-based electrocatalysts to optimize the catalytic performance for the oxygen evolution reaction (OER) is increasingly important yet remains challenging. Herein, we develop a strategy of the electronic interaction and tip-enhanced local field to synergistically tune the surface reconstruction. As a demonstration, a heterostructure catalyst comprising an FeCo2S4 hollow nanoneedle decorated with MoO3 nanoparticles (MoO3@FeCo2S4) at the tip is constructed. The combined theoretical and in situ X-ray absorption investigations indicate that the abundant Co-O-Mo motifs at the interface improve the electron transfer, facilitating the surface reconstruction into Co(Fe)OOH-MoO3. Meanwhile, the sharp tip of the hollow nanoneedles enhances the local electric field and increases the pH near the tip to promote the formation of active CoOOH. Accordingly, the as-constructed MoO3@FeCo2S4 shows a low overpotential of 277 mV at a current density of 100 mA cm-2 during the alkaline OER and maintains stable operation at 200 mA cm-2 for 100 h. This work not only provides insights for the rational regulation of surface reconstruction but also highlights the important integration of the electronic interaction with a local environment to design advanced transition-metal-based catalysts.

Rational design and integration of benzenoid and nonbenzenoid carbon frameworks enable the construction of low-dimensional carbon nanostructures with unconventional topologies and tailored electronic properties. Here, we demonstrate the on-surface synthesis of nanosized pentaheptite (NPH), a nonbenzenoid molecular carbon consisting of equal numbers of penta-heptagonal units, arising from the strategic precursor design and the inherent structural versatility of carbon skeletons. The as-synthesized NPH adopts a C2h symmetric configuration with largely compensated intramolecular charge polarization, while benzenoid units can be incorporated into the intrinsic penta-heptagonal framework via two possible pathways: an intramolecular Stone-Wales-like skeletal rearrangement and a process involving azulene-naphthalene rearrangements, forming a transformed pentaheptite (T-NPH), as supported by density functional theory simulations. Such a transformation breaks skeletal symmetry, leading to intramolecular charge redistribution and electrostatic asymmetry, as revealed by local probe microscopy measurements and corroborated by density functional theory calculations. Our work highlights the role of skeletal topology rearrangements in governing the local electrostatic properties of nonbenzenoid carbon nanostructures, offering insights into polarity-related electrostatic effects in nonbenzenoid molecular carbons.