Owing to abundant polar groups and good lithiophilicity, protein materials regain interest for application in lithium metal batteries (LMBs). Current proteins with an αconformation for modifying lithium (Li) anodes possess typically poor mechanical properties, and there is therefore a significant need for advanced protein materials. Herein, a lysozyme-modified layer is coated onto the poly(vinylidene fluoride) electrospun mat for high mechanical strength and uniform Li-ion flux. The lysozyme membrane can regulate Li + deposition behavior due to complete β-sheet configuration, high lithiophilicity sulfhydryl groups, and columnar nanopores. As a result, the lysozyme-modified Li metal anode exhibits a high stability performance of Li−Li symmetric cells (2800 h) and Li-LiFePO 4 full cell (1450 cycles). Our strategy pushes the protein with β-sheet configuration toward the applications of next-generation LMBs.