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Achieving structural reversibility under long\u2010term cycling remains a central challenge. Here, we show that tuning the electrolyte solvation environment can directly stabilize Mn redox chemistry and lattice evolution in mild\u2010aqueous Zn||\u03b5\u2010MnO\n                    <jats:sub>2<\/jats:sub>\n                    batteries. Using dimethyl sulfoxide (DMSO) as a co\u2010solvent to lower water activity and reorganize the solvation structure, we reveal through operando X\u2010ray diffraction that the modified electrolyte promotes reversible Zn\n                    <jats:sup>2+<\/jats:sup>\n                    intercalation despite slower transport kinetics. Complementary X\u2010ray photoelectron spectroscopy shows that conventional aqueous electrolytes induce strong Mn\u2010valence gradients between surface and bulk, whereas DMSO suppresses these gradients and maintains uniform redox states. Collectively, these results demonstrate that electrolyte solvation engineering can mitigate parasitic reactions and enable structurally reversible MnO\n                    <jats:sub>2<\/jats:sub>\n                    redox processes, establishing a holistic pathway to enhance the long\u2010term stability of mild\u2010aqueous Zn\u2010based batteries.\n                  <\/jats:p>","DOI":"10.1002\/smll.74927","type":"journal-article","created":{"date-parts":[[2026,8,8]],"date-time":"2026-08-08T06:24:54Z","timestamp":1786170294000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["Coupled Role of Zn\n                    <sup>2+<\/sup>\n                    Reversibility and Reduced Water Activity in Achieving Stable Mild\u2010Aqueous Zn||MnO\n                    <sub>2<\/sub>\n                    Batteries"],"prefix":"10.1002","volume":"22","author":[{"ORCID":"https:\/\/orcid.org\/0000-0002-0954-5803","authenticated-orcid":false,"given":"Varun R.","family":"Kankanallu","sequence":"first","affiliation":[{"name":"Department of Materials Science and Chemical Engineering Stony Brook University  Stony Brook New York USA"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0009-0008-3437-1228","authenticated-orcid":false,"given":"Adesanmi","family":"Adeniyi","sequence":"additional","affiliation":[{"name":"Department of Materials Science and Chemical Engineering Stony Brook University  Stony Brook New York USA"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-0575-2987","authenticated-orcid":false,"given":"Jianming","family":"Bai","sequence":"additional","affiliation":[{"name":"National Synchrotron Light Source II Brookhaven National Laboratory  Upton New York 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Photon Sciences Directorate Brookhaven National Laboratory  Upton New York USA"},{"name":"Department of Chemistry Stony Brook University  Stony Brook New York USA"},{"name":"Institute of Sustainability Electrification, and Energy, Energy (I:SEE) Stony Brook University  Stony Brook New York USA"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Mingyuan","family":"Ge","sequence":"additional","affiliation":[{"name":"National Synchrotron Light Source II Brookhaven National Laboratory  Upton New York USA"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-4445-2159","authenticated-orcid":false,"given":"Yu\u2010chen Karen","family":"Chen\u2010Wiegart","sequence":"additional","affiliation":[{"name":"Department of Materials Science and Chemical Engineering Stony Brook University  Stony Brook New York USA"},{"name":"National Synchrotron Light Source II Brookhaven National Laboratory  Upton New York 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