Lithium metal anode (LMA) is puzzled by the serious issues corresponding to infinite volume change and notorious lithium dendrite during long‐term stripping/plating process. Herein, the transition metal nitrides array with outstanding lithiophilicity, including CoN, VN, and Ni3N, are decorated onto carbon framework as “nests” to uniform Li nucleation and guide Li metal deposition. These transition metal nitrides with excellent conductivity can guarantee the fast electron transport, therefore maintain a stable interface for Li reduction. In addition, the designed multi‐dimensional structure of metal nitride array decorated carbon framework can effectively regulate the growth of Li metal during the stripping/plating process. Of note, attributing to the lattice‐matching between CoN and Li metal, the composite Li/CoN@CF anode exhibits ultra‐stable cycling performance in symmetrical cells (over 4000 h@1 mA cm−2 with 1 mAh cm−2 and 1000h@20 mA cm−2 with 20 mAh cm−2). The assembled full cells based on Li/CoN@CF composite anode, LiFePO4 or S as cathodes, deliver excellent cycling stability and rate capability. This strategy provides an effective approach to develop a stable lithium metal anode for lithium metal batteries.
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