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We present a molecularly engineered polyoxometalate\u2010functionalized mesoporous metal\u2013organic framework (meso\u2010MOF@POM) nanoarchitecture that simultaneously reinforces the hydrogel network and enhances interfacial charge kinetics. The meso\u2010MOF serves as a hierarchical scaffold with multiscale channels for polymer anchoring, while the sub\u2010nanometer Keggin\u2010type POM layer creates abundant redox\u2010mediated electron transfer pathways. Upon integration of meso\u2010MOF@POM into a dual\u2010network poly(acrylic acid)\/polyacrylamide hydrogel, the composite hydrogel enables high stretchability (&gt;1000% strain), minimal electrical creep (&lt;0.13% s\n                    <jats:sup>\u22121<\/jats:sup>\n                    @100% strain), and good cyclic durability (&gt;3000 cycles). Crucially, the engineered organic\u2013inorganic interface endows the hydrogel with excellent pseudocapacitive charge\u2010transfer kinetics, which achieves low skin\u2013electrode impedance (64 k\u03a9 at 1\u00a0Hz vs. 287 k\u03a9 at 1\u00a0Hz for Ag\/AgCl gel). As a result, the skin\u2010interfacing electrode enables high\u2010fidelity recording of on\u2010skin electrophysiological signals, including electrocardiogram, electromyogram, and electrooculogram, with an enhanced signal\u2010to\u2010noise ratio (e.g., 23.8\u00a0dB for ECG vs. 21.3\u00a0dB for Ag\/AgCl gel). This work provides a novel fabrication strategy for highly conductive interfaces, enabling long\u2010term applications in wearable health monitors and human\u2013machine interfaces.\n                  <\/jats:p>","DOI":"10.1002\/adma.74792","type":"journal-article","created":{"date-parts":[[2026,8,31]],"date-time":"2026-08-31T10:42:43Z","timestamp":1788172963000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["Pseudocapacitive Charge\u2010Transfer Interface via Polyoxometalate\u2010Functionalized Mesoporous MOF for Highly Reliable and High\u2010Fidelity Bioelectronic Hydrogels"],"prefix":"10.1002","volume":"38","author":[{"given":"Wenjie","family":"Dong","sequence":"first","affiliation":[{"name":"State Key Laboratory of High Performance Ceramics Shanghai Institute of Ceramics Chinese Academy of Sciences Shanghai P. R. China"},{"name":"Center of Materials Science and Optoelectronics Engineering University of Chinese Academy of Sciences Beijing P. R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Chen","family":"Luan","sequence":"additional","affiliation":[{"name":"State Key Laboratory of High Performance Ceramics Shanghai Institute of Ceramics Chinese Academy of Sciences Shanghai P. R. China"},{"name":"Zhejiang Key Laboratory of Industrial Solid Waste Thermal Hydrolysis Technology and Intelligent Equipment Huzhou University Huzhou P. R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0009-0003-4100-5211","authenticated-orcid":false,"given":"Yao","family":"Dai","sequence":"additional","affiliation":[{"name":"State Key Laboratory of High Performance Ceramics Shanghai Institute of Ceramics Chinese Academy of Sciences Shanghai P. R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Jin","family":"Yang","sequence":"additional","affiliation":[{"name":"State Key Laboratory of High Performance Ceramics Shanghai Institute of Ceramics Chinese Academy of Sciences Shanghai P. R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Jiaqi","family":"Wang","sequence":"additional","affiliation":[{"name":"State Key Laboratory of High Performance Ceramics Shanghai Institute of Ceramics Chinese Academy of Sciences Shanghai P. R. China"},{"name":"Zhejiang Key Laboratory of Industrial Solid Waste Thermal Hydrolysis Technology and Intelligent Equipment Huzhou University Huzhou P. R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-4506-2689","authenticated-orcid":false,"given":"Zhanqiang","family":"Liu","sequence":"additional","affiliation":[{"name":"Zhejiang Key Laboratory of Industrial Solid Waste Thermal Hydrolysis Technology and Intelligent Equipment Huzhou University Huzhou P. R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Huanqian","family":"Zhang","sequence":"additional","affiliation":[{"name":"State Key Laboratory of Functional Materials for Informatics Shanghai Institute of Microsystem and Information Technology Chinese Academy of Sciences Shanghai P. R. 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