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Coating Zr‐based metallic glass, Zr53Cu31Ni11Al5 (Zr‐MG), on a Cu current collector (CC) and Li metal anode (LMA) significantly improves the cycle performance of both types of Li‐ion batteries, namely, anode‐free Li‐ion batteries (AFLBs) and Li metal batteries (LMB). The inherent isotropy and homogeneity of the Zr‐MG significantly improve the surface uniformity of the CC and LMA. A 12 nm‐thick Zr‐MG...