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Here, we report a molecule\u2010reconstruction strategy to regulate Li\n                    <jats:sup>+<\/jats:sup>\n                    solvation by exploiting the amplified steric hindrance generated during in situ polymerization of isobutyl methacrylate (IBMA). Covalently linking IBMA monomers into macromolecular chains increases steric bulk around polar ester groups, reduces the electron cloud density of carbonyl oxygen, weakens Li\n                    <jats:sup>+<\/jats:sup>\n                    \u2010polymer coordination, and drives a transition from solvent\u2010dominated to anion\u2010rich solvation even at low salt concentrations. With TTE serving as a \u201cmolecular lubricant\u201d, the gel solid\u2010state DEE\u2010PIBMA electrolyte achieves a room\u2010temperature ionic conductivity of 1.77\u00a0mS cm\n                    <jats:sup>\u22121<\/jats:sup>\n                    and practical high\u2010voltage stability to \u223c4.7\u00a0V, as confirmed by floating tests. Gel solid\u2010state Li||NCM811 cells retain 81.8% of their initial capacity after 500 cycles at 0.5\u00a0C, while pouch cells operate stably with an energy density of 386.1\u00a0Wh kg\n                    <jats:sup>\u22121<\/jats:sup>\n                    . These results highlight macromolecular backbone engineering as a general design principle for regulating solvation structures and interfacial chemistry in high\u2010energy LMBs.\n                  <\/jats:p>","DOI":"10.1002\/anie.5513729","type":"journal-article","created":{"date-parts":[[2026,9,29]],"date-time":"2026-09-29T06:02:20Z","timestamp":1790661740000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["Monomer Molecule Reconstruction Engineered Heterogeneous Lithium\u2010Ion Solvation for High\u2010Performance Lithium\u2010Metal Batteries"],"prefix":"10.1002","author":[{"given":"Yanxin","family":"Jiang","sequence":"first","affiliation":[{"name":"College of Materials Science and Chemical Engineering Harbin Engineering University  Harbin P.R. China"},{"name":"Department of Mechanical and Energy Engineering Southern University of Science and Technology  Shenzhen P.R. 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China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0009-0009-0077-5176","authenticated-orcid":false,"given":"Zhiqiang","family":"Yang","sequence":"additional","affiliation":[{"name":"Department of Mechanical and Energy Engineering Southern University of Science and Technology  Shenzhen P.R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Mingnan","family":"Song","sequence":"additional","affiliation":[{"name":"Department of Mechanical and Energy Engineering Southern University of Science and Technology  Shenzhen P.R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-0377-1228","authenticated-orcid":false,"given":"Liang","family":"Wang","sequence":"additional","affiliation":[{"name":"Centre For Catalysis and Clean Energy School of Environment and Science Griffith University  Gold Coast Queensland Australia"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0009-0000-9301-5081","authenticated-orcid":false,"given":"Chunling","family":"Zhu","sequence":"additional","affiliation":[{"name":"College of Materials Science and Chemical Engineering Harbin Engineering University  Harbin P.R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-2842-2355","authenticated-orcid":false,"given":"Guiling","family":"Wang","sequence":"additional","affiliation":[{"name":"College of Materials Science and Chemical Engineering Harbin Engineering University  Harbin P.R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-2419-6928","authenticated-orcid":false,"given":"Jiaxin","family":"Yao","sequence":"additional","affiliation":[{"name":"College of Materials Science and Chemical Engineering Harbin Engineering University  Harbin P.R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-3824-7693","authenticated-orcid":false,"given":"Shi\u2010Xue","family":"Dou","sequence":"additional","affiliation":[{"name":"Institute of Energy Materials Science (IEMS) University of Shanghai for Science and Technology  Shanghai P.R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-9240-5686","authenticated-orcid":false,"given":"Yiju","family":"Li","sequence":"additional","affiliation":[{"name":"Department of Mechanical and Energy Engineering Southern University of Science and Technology  Shenzhen P.R. 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