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Here, inspired by the hierarchical architecture of organisms like the lotus leaf, a micro\u2013nano hierarchical composite electrolyte was fabricated via in situ growth of a bifunctional metal\u2013organic framework (F&amp;OH\u2010ZIF\u20108) on a cellulose acetate (CA) substrate. The micro\u2010 and nano\u2010sized F&amp;OH\u2010ZIF\u20108 crystals have the same composition but exhibit different size\u2010dependent advantages. The micro\u2010sized crystals provide greater structural continuity and mechanical support, whereas the nano\u2010sized crystals offer more accessible polar sites and interfacial regions for Li\n                    <jats:sup>+<\/jats:sup>\n                    coordination and transport. Their cooperative integration suppresses dendrite penetration and stabilizes the electrode\/electrolyte interphases while facilitating Li\n                    <jats:sup>+<\/jats:sup>\n                    transport. An outstanding SSE with a room\u2010temperature ionic conductivity of 2.9 \u00d7 10\n                    <jats:sup>\u22123<\/jats:sup>\n                    S cm\n                    <jats:sup>\u22121<\/jats:sup>\n                    , a lithium\u2010ion transference number of 0.61, and a wide electrochemical stability window extending to 5.5 V was obtained by this strategy, resulting in Li||NCM811 full cells achieving a high\u2010capacity retention of 80.9% after 300 cycles at 1C under a high cut\u2010off voltage of 4.6 V. This strategy of transforming existing commercialized ordinary membrane materials into more valuable electrolyte membranes has extremely high practical significance.\n                  <\/jats:p>","DOI":"10.1002\/adma.75227","type":"journal-article","created":{"date-parts":[[2026,10,1]],"date-time":"2026-10-01T04:23:35Z","timestamp":1790828615000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["Micro\u2013Nano Hierarchical Structure From In Situ Functionalized MOFs Enables High\u2010Performance High\u2010Voltage Electrolytes"],"prefix":"10.1002","author":[{"given":"Yixian","family":"Xiao","sequence":"first","affiliation":[{"name":"Institute for Advanced Materials and Technology University of Science and Technology Beijing  Beijing P. R. 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