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To overcome this issue, we design a novel composite Poly(ionic liquid)s based solid electrolyte (CPLE) through the synergistic integration of a main\u2010chain imidazolium\u2010based PIL backbone and a metal\u2010organic framework (MOF\u20105). The main\u2010chain PIL architecture intrinsically mitigate strong intermolecular ionic interactions, while MOF\u20105 framework acts as a multi\u2010functional filler that strongly immobilizes TFSI\n                    <jats:sup>\u2212<\/jats:sup>\n                    anions via Lewis acid\u2010base interactions. This dual\u2010anchoring strategy effectively promotes Li salt dissociation, provides additional ion transport pathways, and remarkably enhance the Li\n                    <jats:sup>+<\/jats:sup>\n                    transference number. Consequently, the CPLE achieves a high room\u2010temperature ionic conductivity of 1.4\u00a0mS\u00a0cm\n                    <jats:sup>\u2212<\/jats:sup>\n                    <jats:sup>1<\/jats:sup>\n                    , an exceptional Li\n                    <jats:sup>+<\/jats:sup>\n                    transference number of 0.7, and a widened electrochemical stability window up to 4.6\u00a0V. The strong interfacial interaction between the PIL and MOF\u20105 also reinforces mechanical strength (1.9\u00a0MPa tensile strength). This unique synergy enables outstanding interfacial stability: Li||Li symmetric cells cycle stably for over 2000\u00a0h at 0.1\u00a0mA\u00a0cm\n                    <jats:sup>\u2212<\/jats:sup>\n                    <jats:sup>2<\/jats:sup>\n                    , and Li||LiFePO\n                    <jats:sub>4<\/jats:sub>\n                    full cells retain 80% capacity after 700 cycles at 1 C. Crucially, the CPLE is compatible with high\u2010voltage LiNi\n                    <jats:sub>0.8<\/jats:sub>\n                    Co\n                    <jats:sub>0.1<\/jats:sub>\n                    Mn\n                    <jats:sub>0.1<\/jats:sub>\n                    O\n                    <jats:sub>2<\/jats:sub>\n                    cathodes.\n                  <\/jats:p>","DOI":"10.1002\/smtd.70800","type":"journal-article","created":{"date-parts":[[2026,6,30]],"date-time":"2026-06-30T07:06:35Z","timestamp":1782803195000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["Synergistic Anion Confinement in a Poly(Ionic Liquid)\/MOF Composite Electrolyte Decouples Ionic Conductivity and Mechanical Strength for High\u2010Performance Solid\u2010State Lithium Metal Batteries"],"prefix":"10.1002","volume":"10","author":[{"given":"Ziyan","family":"Liu","sequence":"first","affiliation":[{"name":"College of Chemistry State Key Laboratory of Chemical Resource Engineering Beijing University of Chemical Technology  Beijing China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Li","family":"Yu","sequence":"additional","affiliation":[{"name":"College of Chemistry State Key Laboratory of Chemical Resource Engineering Beijing University of Chemical Technology  Beijing China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Weifan","family":"Wang","sequence":"additional","affiliation":[{"name":"College of Chemistry State Key Laboratory of Chemical Resource Engineering Beijing University of Chemical Technology  Beijing China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Mengchao","family":"Li","sequence":"additional","affiliation":[{"name":"College of Chemistry State Key Laboratory of Chemical Resource Engineering Beijing University of Chemical Technology  Beijing 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