Nonuniform nucleation is one of the major reasons for the dendric growth of metallicl ithium, whichl eads to intractable problems in the efficiency,r eversibility,a nd safety in Li-based batteries. To improve the deposition of metallic Li on Cu substrates, herein, af reestandingc urrent collector (NGDY@CuNW) is formed by coatingpyridinic nitrogen-doped graphdiyne (NGDY) nanofilms on 3D Cu nanowires (CuNWs). Theoretical predictions reveal that the introductiono fn itrogen atoms in the 2D GDY can enhance the binding energy between the Li atom and GDY,t herefore improving thel ithiophilicity on the surface for uniform lithium nucleation and deposition. Accordingly,the deposited metallic Li on the NGDY@CuNW electrode exhibitsadendrite-free morphology,r esultingi ns ignificant improvements in terms of the reversibility with ah igh coulombic efficiency (CE) and along lifespana thigh currentd ensity.Our research provides an efficient methodt oc ontrol the surfacep roperty of Cu, which also will be instructive for other metal batteries.Supporting information and the ORCID identification number(s) for the author(s) of this articlecan be found under: https://doi.