The rapid development of modern society have stimulated intensive research on advanced energy storage systems with high energy density and high safety to meet the rising demand for large-scale energy storage systems, such as electric vehicles and smart grid. As one of the most promising anode candidates, Li metal has received much attention owing to its ultrahigh theoretical capacity (3860 mAh g −1 ), the lowest electrochemical potential (−3.040 V vs standard hydrogen electrode) and low density (0.534 g cm −3 ). [1,2] Nevertheless, the practical large-scale application of Li metal has long been fettered by serious safety challenges caused by the uncontrollable Li deposition during Li plating/stripping process, resulting in lithium dendrite growth which could penetrate the separator leading to battery failureThe large-scale implementation of lithium metal batteries (LMBs) has long been plagued by the uncontrollable Li deposition triggered safety issues. Herein, a lithiophilic three-dimensional Li anode scaffold, which is prepared by molten Li infusion aided by confined growth of low-cost Zn clusters, is rationally constructed for high-performance LMBs. Owing to the synergy of the carbon host and the effective regulation from the Zn nanoclusters, the large volumetric change of Li metal is well mitigated and shows a smooth and dendrite-free behavior. The Li anode scaffold can deliver much improved Coulombic efficiency, superior rate performance, and long cycle lifespan with much lower voltage polarization. Furthermore, the half cells of Li anode scaffold paired with LiFePO 4 /LiCoO 2 /sulfur can achieve a higher specific capacity and longer stable cycling life than those with conventional Li foil. The Li|LFP cells can achieve a stable cycling over 250 cycles at 1C with a higher capacity retention of ≈90.8%, and a higher initial discharge capacity of 924.6 mAh g −1 with a high capacity retention over 300 cycles can also be obtained in Li|S cells at 1C. This work demonstrates a cost-effective and scalable strategy for stable Li metal anode toward next-generation and high-performance LMBs. www.advancedsciencenews.com