Lithium metal batteries have recently emerged as alternative energy storage systems beyond lithium-ion batteries. However, before this kind of batteries can become a viable technology, the critical issues of the Li anodes, like dendrites growth and low Coulombic efficiency (CE), need to be conquered. Herein, lithiophilic Cu-metal-organic framework thin layer (Cu-MOF TL) is in situ grown on the surface of Cu foil by a facile immersion strategy to construct a multifunctional current collector. Profiting from the high electrical conductivity and unique porous structure, the Cu-MOF TL with high affinity to electrolyte can provide uniform nucleation sites and promote homogeneous Li+ flux, as a result, radically restrain the Li dendrite growth, leading to stable Li plating/striping behaviors. The modified current collector enables Li plating/stripping with a prominent CE (∼97.1%) and a stable lifetime (∼2500 h). Importantly, the synthesis method can be easily large-scale production in a series of organic solvents.