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Here, we report a bias\u2010responsive S\u2010scheme heterojunction that dynamically couples nonequilibrium electron redistribution with interfacial water activation during operation. Using a MoN\/NiCoN model system, in situ x\u2010ray absorption spectroscopy (XAS) reveals a cathodic\u2010bias\u2010induced reversal of interfacial electron transfer relative to the equilibrium state, leading to progressive electron enrichment at the catalytic interface. In situ infrared spectroscopy reveals potential\u2010dependent restructuring of the interfacial water environment associated with this electronic redistribution, transforming strongly and intermediately hydrogen\u2010bonded water into catalytically active free or weakly hydrogen\u2010bonded species. Ab initio molecular dynamics simulations further reveal accelerated hydrogen\u2010bond exchange kinetics, shortened hydrogen\u2010bond lifetimes, and a more adaptive dipole orientation at the MoN\/NiCoN interface, providing molecular\u2010level evidence for dynamic water\u2010network reorganization. Ionic\u2010liquid\u2010based experiments further demonstrate that this restructuring originates from electronically driven interfacial activation rather than bulk water availability. Consequently, water dissociation and hydrogen evolution kinetics are synergistically accelerated, enabling ultralow overpotentials in real seawater and high solar\u2010to\u2010hydrogen (STH) conversion efficiency. This work establishes dynamic S\u2010scheme heterojunctions as a general strategy for electronically programmable interfacial reaction environments in electrocatalysis.<\/jats:p>","DOI":"10.1002\/adma.75083","type":"journal-article","created":{"date-parts":[[2026,9,21]],"date-time":"2026-09-21T04:50:40Z","timestamp":1789966240000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["Bias\u2010Responsive S\u2010Scheme Heterojunctions Reconfigure Interfacial Water for Efficient Seawater Hydrogen Evolution"],"prefix":"10.1002","author":[{"ORCID":"https:\/\/orcid.org\/0009-0003-6543-0490","authenticated-orcid":false,"given":"Zhenrui","family":"Ni","sequence":"first","affiliation":[{"name":"Laboratory of Solar Fuel Faculty of Materials Science and Chemistry China University of Geosciences  Wuhan P. R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-1892-0844","authenticated-orcid":false,"given":"Ruchun","family":"Li","sequence":"additional","affiliation":[{"name":"Yunnan Key Laboratory of Modern Separation Analysis and Substance Transformation College of Chemistry and Chemical Engineering Yunnan Normal University  Kunming P. R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-9186-9080","authenticated-orcid":false,"given":"Olim","family":"Ruzimuradov","sequence":"additional","affiliation":[{"name":"Alfraganus University  Tashkent Uzbekistan"},{"name":"Turin Polytechnic University  Tashkent Uzbekistan"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-0627-5449","authenticated-orcid":false,"given":"Khayit","family":"Turaev","sequence":"additional","affiliation":[{"name":"Termez State University  Termez Uzbekistan"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-9420-0702","authenticated-orcid":false,"given":"Weilai","family":"Yu","sequence":"additional","affiliation":[{"name":"Deparmtent of Chemical Engineering and Applied Chemistry University of Toronto  Toronto ON Canada"},{"name":"Deparmtent of Chemistry The Hong Kong University of Science and Technology  Hong Kong SAR P. R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-2551-3702","authenticated-orcid":false,"given":"Panyong","family":"Kuang","sequence":"additional","affiliation":[{"name":"Laboratory of Solar Fuel Faculty of Materials Science and Chemistry China University of Geosciences  Wuhan P. R. 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