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Herein, we report an active layer of 2,4,6\u2013trihydroxy benzene sulfonyl fluorine on copper substrate that induces oriented Li<jats:sup>+<\/jats:sup> deposition and generates highly crystalline solid\u2010electrolyte interphase (SEI) to achieve high\u2010performance LMBs. The lithiophilic \u2212SO<jats:sub>2<\/jats:sub><jats:sup>\u2212<\/jats:sup> groups of highly crystalline SEI accept the rapidly transported Li<jats:sup>+<\/jats:sup> ions and form a dense inner layer of LiF and Li<jats:sub>3<\/jats:sub>N, which regulate Li<jats:sup>+<\/jats:sup> plating morphology along the (110) crystal surface toward dendrite\u2010free Li anode. Thus, Li||Cu cells with lithiophilic SEI achieve an average deposition efficiency of 99.8\u2009% after 700\u2005cycles, and Li||Li cells operate well for 1100\u2005h. 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