AbstractThe development and application of rechargeable aqueous zinc‐ion batteries are seriously hindered by the problems of corrosion and dendrite growth on Zn metal anodes. Herein, a polyporous 3D zinc framework coupled with a zincophilic ZnSe overlayer (3D‐Zn@ZnSe) is synchronously obtained by one‐step electrochemical scanning, which precisely repairs intrinsic defects of the Zn foil surface and remodels the electrolyte/anode interface. The 3D‐Zn host formed by the pioneering electro‐oxidation significantly reduces the local current densities and facilitates adapting to the volume change during the plating/stripping. Meanwhile, the ZnSe overlayer obtained by electro‐deposition restrains the side reactions and promotes efficient desolvation, resulting in the acceleration of the deposition kinetics of Zn²⁺ on the zinc anode. As a result, the anodes present an enhanced cycling stability of zinc plating/stripping for over 2000 h with low overpotential, and the assembled 3D‐Zn@ZnSe||V₂O₅ cell retains 90.63% of its original capacity after 8500 cycles. The one‐step fabrication of polyporous interfaces with a zincophilic overlayer presents a promising strategy on improving the stability and reversibility of zinc anode for zinc‐based batteries.