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In this study, it is discovered that a distinct interphase can be spontaneously formed between the aqueous and organic phases through the synergy of amphiphilic monomers, Hofmeister effects, and phase partitioning. This aqueous\u2013organic, mixed\u2010solvent region boosts ion transfer by smoothing solvation change across phases, resulting in an order\u2010of\u2010magnitude increase in overall conductivity over biphasic counterparts without such an interphase. Meanwhile, compartmentalized organo\u2010 and hydrogel domains decouple anodic and cathodic interfacial chemistries. Demonstrated in zinc metal batteries, this biphasic gel electrolyte thermodynamically stabilizes zinc metal anodes and inhibits parasitic ion crossover, while also enabling high\u2010rate operation comparable to aqueous systems. Accordingly, Zn||Zn symmetric cells demonstrate &gt;3,600\u00a0h stable cycling at 5\u00a0mA cm\n                    <jats:sup>\u22122<\/jats:sup>\n                    and 5\u00a0mAh cm\n                    <jats:sup>\u22122<\/jats:sup>\n                    , and MnO\n                    <jats:sub>2<\/jats:sub>\n                    ||Zn full cells show high capacity retention after &gt;3,000 cycles at 10\u00a0A g\n                    <jats:sup>\u22121<\/jats:sup>\n                    . Overall, the findings establish organizing phase and solvation chemistry as a general materials design principle toward advanced electrolyte systems for high\u2010power, long\u2010duration electrochemical energy storage.\n                  <\/jats:p>","DOI":"10.1002\/adma.74466","type":"journal-article","created":{"date-parts":[[2026,8,5]],"date-time":"2026-08-05T12:09:27Z","timestamp":1785931767000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":1,"title":["A Hydro\u2013Organo Biphasic Gel Electrolyte for Decoupled Interfacial Stability and Fast Ion Transport in Zinc Metal Batteries"],"prefix":"10.1002","volume":"38","author":[{"given":"Tianrui","family":"Zheng","sequence":"first","affiliation":[{"name":"Materials Science and Engineering Program, Texas Materials Institute The University of Texas at Austin  Austin Texas USA"},{"name":"Walker Department of Mechanical Engineering The University of Texas at Austin  Austin Texas 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