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Conventional approaches typically involve tuning electrolyte compositions to indirectly generate SEIs dominated by organic or inorganic components. However, organic\u2010rich SEI fails to inhibit the growth of Li dendrites, compromising sluggish Li\n                    <jats:sup>+<\/jats:sup>\n                    kinetics, and inorganic\u2010rich SEI suffers from mechanical brittleness at low temperatures, resulting in inadequate interfacial mechanical stability. Herein, we introduce a siloxane\u2010based elastomeric coating on the Li anode surface by leveraging its intrinsic solvent phobicity to achieve selective ion conduction, facilitating the formation of a LiF\u2010rich inner SEI, which synergizes with the elastomer to construct a double\u2010layer organic\u2010inorganic SEI. Theoretical calculations and experimental results demonstrate that such a double\u2010layer SEI combines mechanical flexibility enabled by organic components with promoted Li\n                    <jats:sup>+<\/jats:sup>\n                    transport imparted by inorganic components, synergistically improving the cycling stability of LMBs under low\u2010temperature conditions. The target LMBs paired with industrial\u2010standard NCM811 cathodes deliver 99% capacity retention over 300 cycles at \u201325\u00b0C. Unlike indirect electrolyte modification approaches, our method enables direct manipulation of SEI structures and is compatible with various electrolyte systems.\n                  <\/jats:p>","DOI":"10.1002\/adma.73917","type":"journal-article","created":{"date-parts":[[2026,7,3]],"date-time":"2026-07-03T08:54:20Z","timestamp":1783068860000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":1,"title":["A Selective\u2010Transport Elastomeric Coating Regulating Hierarchical Solid Electrolyte Interphase for Low\u2010Temperature Lithium\u2010Metal Batteries"],"prefix":"10.1002","volume":"38","author":[{"given":"Hang","family":"Ding","sequence":"first","affiliation":[{"name":"State Key Laboratory of Organic\u2010Inorganic Composites, College of Materials Science and Engineering Beijing University of Chemical Technology  Beijing P. R. 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China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Jingren","family":"Gou","sequence":"additional","affiliation":[{"name":"State Key Laboratory of Organic\u2010Inorganic Composites, College of Materials Science and Engineering Beijing University of Chemical Technology  Beijing P. R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Ming","family":"Tian","sequence":"additional","affiliation":[{"name":"State Key Laboratory of Organic\u2010Inorganic Composites, College of Materials Science and Engineering Beijing University of Chemical Technology  Beijing P. R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Peng\u2010Fei","family":"Cao","sequence":"additional","affiliation":[{"name":"State Key Laboratory of Organic\u2010Inorganic Composites, College of Materials Science and Engineering Beijing University of Chemical Technology  Beijing P. R. 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