Metallic zinc is attractive anode material of rechargeable aqueous Zn-based batteries due to its ambient stability, high volumetric capacity, and abundant reserves. Nonetheless, Zn anodes suffer from issues such as low coulombic efficiency (CE), large polarization and dendrite formation. Herein, uniform Zn electrodeposition is reported on carbon substrates by selective nitrogen doping. Combined experimental and theoretical investigations demonstrate that pyrrolic and pyridinic nitrogen doped in carbon play beneficial effect as zinc-philic sites to direct nucleation and growth of metallic Zn, while negligible effect is observed for graphite nitrogen in Zn plating. The carbon cloth with modified amount of doped pyrrolic and pyridinic nitrogen stabilizes Zn plating/stripping with 99.3% CE after 300 cycles and significantly increases the deliverable capacity at high depth of charge and discharge compared to undoped carbon substrate and Zn foil. This work provides a better understanding of heteroatom doping effect in design and preparation of stable 3D carbon-supported zinc anode.