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Herein, we report a polyrotaxane\u2010assembled supramolecular semi\u2010interpenetrating network electrolyte (SSNE), synthesized through in situ polymerization of polyrotaxane with crosslinked polydioxolane (PDOL). The key innovations of this architecture are threefold: it creates hierarchical ion\u2010conduction pathways, introduces Lewis acid sites, and imposes spatial confinement within a polyrotaxane framework. Through host\u2010guest interactions, these elements synergistically decouple the transport of Li\n                    <jats:sup>+<\/jats:sup>\n                    ions from the migration of anions. The SSNE exhibits impressive room\u2010temperature ionic conductivity of 0.18 mS cm\n                    <jats:sup>\u2212<\/jats:sup>\n                    <jats:sup>1<\/jats:sup>\n                    and Li\n                    <jats:sup>+<\/jats:sup>\n                    transference number ( &gt; 0.73). Furthermore, fluorine\u2010 and boron\u2010functionalized polyrotaxane stabilizes the electrode\u2013electrolyte interphase and extends the electrochemical window (&gt; 4.9\u00a0V). The full cell prototype comprising the 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                    cathode, the SSNE, and Li foil delivers 81.4% capacity retention after 200 cycles and rate capability up to 2C. Moreover, a 1.2 Ah pouch\u2010format cell operates reliably for 190 cycles at room temperature with a cutoff voltage of 4.5\u00a0V. This study integrates dynamic polyrotaxane chemistry with a semi\u2010interpenetrating polymer electrolyte architecture, offering a molecule\u2010to\u2010system strategy for the development of next\u2010generation high\u2010voltage lithium metal batteries.\n                  <\/jats:p>","DOI":"10.1002\/advs.202521892","type":"journal-article","created":{"date-parts":[[2026,3,8]],"date-time":"2026-03-08T13:14:41Z","timestamp":1772975681000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":1,"title":["Polyrotaxane\u2010Assembled Semi\u2010Interpenetrating Polymer Electrolytes Enabling High\u2010Voltage Lithium Metal Batteries"],"prefix":"10.1002","volume":"13","author":[{"given":"Tianyi","family":"Wang","sequence":"first","affiliation":[{"name":"Shaanxi Key Laboratory of Macromolecular Science and Technology School of Chemistry and Chemical Engineering Northwestern Polytechnical University  Xi'an P. R. 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