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Here, we propose a descriptor\u2010guided dynamic solvation\u2010shell reconstruction strategy for poly(ethylene oxide) (PEO)\u2010based quasi\u2010solid electrolytes by introducing nitrile plasticizers with competitive Li\n                    <jats:sup>+<\/jats:sup>\n                    affinity and fast local Li\n                    <jats:sup>+<\/jats:sup>\n                    diffusivity. These nitrile ligands competitively enter the first Li\n                    <jats:sup>+<\/jats:sup>\n                    solvation shell, weaken persistent Li\n                    <jats:sup>+<\/jats:sup>\n                    \u2010ether oxygen coordination, and shift Li\n                    <jats:sup>+<\/jats:sup>\n                    migration from polymer\u2010cage\u2010confined hopping to ligand\u2010exchange\u2010assisted transport. The optimized electrolyte achieves a room\u2010temperature ionic conductivity of 10.9 mS cm\n                    <jats:sup>\u22121<\/jats:sup>\n                    , nearly three orders of magnitude higher than that of the pristine PEO electrolyte. Meanwhile, the nitrile\u2010containing solvation shell regulates interfacial decomposition pathways, suppresses oxidative PEO degradation in high\u2010voltage Li\u2016NCM811 cells, and promotes the formation of compact cathode electrolyte interphases. Benefiting from simultaneously enhanced bulk Li\n                    <jats:sup>+<\/jats:sup>\n                    transport and high\u2010voltage interfacial stability, the optimized electrolyte enables stable fast\u2010charging cycling and low\u2010temperature operation in Li\u2016NCM811 cells. This work establishes descriptor\u2010guided dynamic first\u2010solvation\u2010shell reconstruction as a molecular design principle for high\u2010conductivity, high\u2010voltage\u2010stable PEO\u2010based quasi\u2010solid electrolytes.\n                  <\/jats:p>","DOI":"10.1002\/anie.3211208","type":"journal-article","created":{"date-parts":[[2026,8,26]],"date-time":"2026-08-26T04:25:56Z","timestamp":1787718356000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":1,"title":["Descriptor\u2010Guided Dynamic Solvation\u2010Shell Reconstruction Enables PEO\u2010Based Polymer Electrolytes With 10.9 mS cm\n                    <sup>\u22121<\/sup>\n                    \u00a0Ionic Conductivity"],"prefix":"10.1002","volume":"65","author":[{"given":"Yutong","family":"Zhai","sequence":"first","affiliation":[{"name":"National &amp; Local United Engineering Laboratory For Power Battery Department of Chemistry Northeast Normal University  Changchun China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Botian","family":"Zheng","sequence":"additional","affiliation":[{"name":"College of Plant Science Jilin University  Changchun China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Ning","family":"Wang","sequence":"additional","affiliation":[{"name":"National &amp; Local United Engineering Laboratory For Power Battery Department of Chemistry Northeast Normal University  Changchun China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Pingbo","family":"Xu","sequence":"additional","affiliation":[{"name":"National &amp; Local United Engineering Laboratory For Power Battery Department of Chemistry Northeast Normal University  Changchun China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Tianzong","family":"Ma","sequence":"additional","affiliation":[{"name":"National &amp; Local United Engineering Laboratory For Power Battery Department of Chemistry Northeast Normal University  Changchun China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Tong","family":"Wu","sequence":"additional","affiliation":[{"name":"Inner Mongolia Engineering Research Center of Lithium\u2010Sulfur Battery Energy Storage College of Chemistry and Materials Science Inner Mongolia Minzu University Tongliao China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Lina","family":"Cong","sequence":"additional","affiliation":[{"name":"National &amp; Local United Engineering Laboratory For Power Battery Department of Chemistry Northeast Normal University  Changchun China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-7653-4071","authenticated-orcid":false,"given":"Haiming","family":"Xie","sequence":"additional","affiliation":[{"name":"National &amp; Local United Engineering Laboratory For Power Battery Department of Chemistry Northeast Normal University  Changchun 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