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Such approaches not only consume significant energy but also provide limited control over polymer network formation, frequently necessitating additional co\u2010solvents or additives to meet mechanical and electrochemical requirements. Herein, we present a solvation regulation strategy that decouples radical polymerization from external energy inputs through solvation\u2010state engineering of the precursor, enabling the rapid (&lt;1 min), spontaneous formation of a polyacrylamide organohydrogel at room temperature. Mechanistically, Zn\n                    <jats:sup>2+<\/jats:sup>\n                    and BF\n                    <jats:sub>4<\/jats:sub>\n                    <jats:sup>\u2212<\/jats:sup>\n                    synergistically reduce the activation barrier for initiator dissociation, while formamide acts as a dynamic solvation shield, suppressing water\u2010induced radical quenching. This solvation\u2010state adjustment also modifies the hydrogen\u2010bonding network, lowers the freezing point to \u221254\u00b0C and enhances mechanical robustness. The optimized microenvironment further mitigates parasitic reactions and zinc dendrite formation. As a result, symmetric Zn||Zn cells maintain stable cycling for over 10\u00a0000 h at \u221240\u00b0C, while flexible Zn\/polyaniline full cells retain reversible capacity over 1000 cycles and exhibit stable performance under repeated mechanical deformation at \u221240\u00b0C. This work demonstrates an energy\u2010efficient, scalable strategy for producing gel electrolytes suitable for aqueous energy storage under extreme conditions.\n                  <\/jats:p>","DOI":"10.1002\/smll.76067","type":"journal-article","created":{"date-parts":[[2026,9,30]],"date-time":"2026-09-30T14:39:26Z","timestamp":1790779166000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["Solvation\u2010Regulated Ultrafast Formation of Organohydrogel Electrolytes for Subzero Flexible Zinc\u2010Ion Batteries"],"prefix":"10.1002","author":[{"given":"Hexian","family":"Ma","sequence":"first","affiliation":[{"name":"School of Materials Science and Engineering Shanghai Jiao Tong University  Shanghai People's Republic of China"},{"name":"Zhangjiang Institute for Advanced Study (ZIAS) Shanghai Jiao Tong University  Shanghai People's Republic of 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