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Although\u00a0existing\u00a0strategies such as \u201cwater\u2010in\u2010salt\u201d and water\u2013organic hybrid electrolytes can widen the electrochemical stability window (ESW), trace water electrolysis still occurs at the interface, leading to gradual pH drift, electrode dissolution, and eventual battery failure. Here, we propose a self\u2010regulating interfacial\u2010boosted electrolyte that effectively addresses these challenges. By introducing phosphate\u2011based components into wide\u2011ESW electrolytes, this design autonomously ensures pH stability via intrinsic buffering capability, spontaneously forms a protective cathode\u2013electrolyte interphase in response to metal\u2010ion dissolution, and reconfigures the ion solvation structure to widen the electrochemical stability window and lowers the interfacial impedance. Demonstrated in a Na\n                    <jats:sub>1<\/jats:sub>\n                    .\n                    <jats:sub>85<\/jats:sub>\n                    Mn[Fe(CN)\n                    <jats:sub>6<\/jats:sub>\n                    ]\n                    <jats:sub>0<\/jats:sub>\n                    .\n                    <jats:sub>97<\/jats:sub>\n                    \u00b72H\n                    <jats:sub>2<\/jats:sub>\n                    O\/\/NaTi\n                    <jats:sub>2<\/jats:sub>\n                    (PO\n                    <jats:sub>4<\/jats:sub>\n                    )\n                    <jats:sub>3<\/jats:sub>\n                    full cell with an energy density of 81.7\u00a0Wh kg\n                    <jats:sup>\u22121<\/jats:sup>\n                    , this electrolyte enables fast charging (75% capacity retention from 1\u00a0C to 80\u00a0C) and ultra\u2010long cycling stability (71% capacity retention after 20\u00a0000 cycles at 80\u00a0C). The strategy offers an effective and generalizable pathway toward high\u2010performance aqueous batteries.\n                  <\/jats:p>","DOI":"10.1002\/adma.74135","type":"journal-article","created":{"date-parts":[[2026,7,14]],"date-time":"2026-07-14T13:03:42Z","timestamp":1784034222000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["Self\u2010Regulating Interfacial\u2010Boosted Electrolytes for Fast\u2010Charging and Long\u2010Life Aqueous Batteries"],"prefix":"10.1002","volume":"38","author":[{"given":"Huan","family":"Li","sequence":"first","affiliation":[{"name":"CAS Key Laboratory of Green Process and Engineering Institute of Process Engineering Chinese Academic of Sciences  Beijing P. R. 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China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Zhao","family":"Chen","sequence":"additional","affiliation":[{"name":"Beijing National Laboratory For Condensed Matter Physics Institute of Physics Chinese Academy of Sciences  Beijing P. R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0009-0002-5582-9046","authenticated-orcid":false,"given":"Bowen","family":"Wang","sequence":"additional","affiliation":[{"name":"Beijing National Laboratory For Condensed Matter Physics Institute of Physics Chinese Academy of Sciences  Beijing P. R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Weiping","family":"Li","sequence":"additional","affiliation":[{"name":"Beijing National Laboratory For Condensed Matter Physics Institute of Physics Chinese Academy of Sciences  Beijing P. R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-9666-8942","authenticated-orcid":false,"given":"Xuefeng","family":"Wang","sequence":"additional","affiliation":[{"name":"Beijing National Laboratory For Condensed Matter Physics Institute of Physics Chinese Academy of Sciences  Beijing P. R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-8430-6474","authenticated-orcid":false,"given":"Yongsheng","family":"Hu","sequence":"additional","affiliation":[{"name":"Beijing National Laboratory For Condensed Matter Physics Institute of Physics Chinese Academy of Sciences  Beijing P. R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-6809-5032","authenticated-orcid":false,"given":"Junmei","family":"Zhao","sequence":"additional","affiliation":[{"name":"CAS Key Laboratory of Green Process and Engineering Institute of Process Engineering Chinese Academic of Sciences  Beijing P. R. China"},{"name":"School of Chemical Engineering University of Chinese Academy of Sciences  Beijing P. R. China"},{"name":"State Key Laboratory of Chemistry and Utilization of Carbon\u2010Based Energy Resources College of Chemistry Xinjiang University  Urumqi P. R. 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