Zinc metal is an important anode material for next-generation energy storage systems. Unfortunately, uncontrollable dendrite growth caused by non-uniform Zn nucleation during the plating process severely restricts their practical applications. Herein, a nitrogen-doped 3D laser scribed graphene (NLSG) with a large surface area and uniform distribution of nucleation sites is used as the interlayer to control Zn nucleation behavior and suppress Zn dendrite growth. The N-containing functional groups in the carbon matrix are highly zincophilic, which can induces uniform nucleation of Zn and guides homogenous Zn deposition. Meanwhile, the large specific area could effectively decrease the local current density, which is more favorable for highly reversible Zn plating/stripping. Benefiting from the superior property, the NLSG demonstrates improved electrochemical performance with high Coulombic efficiency (99.4%) and enhanced cycling performance (200 h). Compared with the bare Zn anodes, the NLSG coated Zn//MnO2 battery demonstrated higher capacity retention (72.3% vs. 59.3%) after 1200 cycles.