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Li metal batteries have attracted extensive research attention because of their extremely high theoretical capacity. However, the commercialization of the Li metal batteries is hindered, as uncontrolled Li dendrites growth leads to safety concerns and a low coulombic efficiency. To suppress Li dendrites growth and achieve dense Li deposition, a lithiophilic 3D Cu host is designed for Li metal anode, in which the nano‐sized Cu is in situ formed with the aid of infused Li metal. The fabricated Li metal anode exhibit a superior electrochemical stability than raw Li metal anode, and compact Li is maintained during cycling. The experimental results and density functional theory calculations demonstrate that the nano‐sized Cu formed on the surface of the skeleton host shows highly exposed Cu (100) and Cu (110) surfaces, which exhibits a strong affinity toward Li, and effectively eliminates the formation of Li dendrites, leading to a dense Li deposition. With the strategy of adjusting exposed surfaces of Cu host, the optimized Li metal anode enhances the electrochemical performance of full cells, and concomitantly demonstrates their potential for future designs of next‐generation Li metal anodes or Li‐free anodes for Li metal batteries. [ABSTRACT FROM AUTHOR]