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Constructing artificial solid electrolyte interface (SEI) is a highly effective approach to overcome the poor reversibility of lithium (Li) metal anodes. Herein, an adhesive and self‐healable supramolecular copolymer, comprising of pendant poly(ethylene oxide) (PEO) segments and ureido‐pyrimidinone (UPy) quadruple hydrogen bonding moieties, is developed as a new protection layer of Li anode by a simple drop‐coating. The protection performance of in‐situ formed LiPEO‐UPy SEI layer is significantly enhanced owing to the strong binding and improved stability arising from a spontaneous reaction between UPy groups with Li metal. Remarkably, an ultrathin (~70 nm) LiPEO‐UPy layer can contribute to stable and dendrite‐free cycling at a high areal c.

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