AbstractRechargeable aqueous zinc‐ion batteries (AZIBs) are one of the most promising post‐lithium battery technologies due to their low cost, high safety, and environmental friendliness. However, their practical development is hindered by the issues of Zn metal anodes, including dendrite growth, passivation, hydrogen evolution and other side reactions. Herein, to circumvent these issues, a facile and universal alloy electrodeposition strategy is proposed to construct a 3D structured ternary Zn alloy artificial interphase layer on Zn foil as an anode for high‐performance AZIBs. The density functional theory (DFT) theoretical calculations, in situ optical visualization and spectroscopic results validate that the zincophilic Zn─Sn─Bi@Zn ternary alloy anode with lower migration energy barrier and weak hydrogen adsorption sites can promote the uniform Zn deposition and suppress hydrogen evolution reactions. The Zn─Sn─Bi@Zn//NH₄V₄O₁₀ full cell demonstrates a high specific capacity 110.4 mAh g⁻¹ even after 10 000 cycles at 5.0 A g⁻¹. Notably, the full cell with a high NH₄V₄O₁₀ cathode loading mass of ≈20.0 mg cm⁻² maintains cyclic stability for 400 cycles. This work proposes an innovative Zn‐based ternary alloy anode methodology as a design strategy for advanced AZIBs and beyond.