Regulating the zinc hydroxide sulfate (ZHS) growth orientation to construct interface layer with electronic insulation and high flux of Zn2+ is an efficient way to suppress parasitic side reactions and Zn dendrite in rechargeable aqueous zinc-ion batteries (ZIBs). Herein, a novel ZnSO4-based electrolyte with dibenzenesulfonimide (BBI) additive is proven able to maintain long-time cycle stabilities of Zn anode. The combination of experimental and precise testing technologies demonstrated that BBI additive can guide a surface-preferred ZHS (001) and Zn (002) crystal plane, as well as prevent the Zn corrosion and dendrite growth to smooth Zn deposition by adjusting the solid-phase interface energy. As a result, the Zn||Cu cells deliver an extended cycling lifespan over 1500 cycles with 99.7 % Coulombic efficiency at the current density of 2 mA cm−2, demonstrating an ultra-stable plating/stripping behavior. More encouragingly, the cyclic stability of Zn-MnO2 battery with the ZnSO4-BBI electrolyte can deliver a specific capacity of ∼165 mAh g−1 after 200 cycles at 1 C. This study clearly elucidates the interface behaviors to stabilize Zn anode, which contributes to a deep insight into the additive regulation mechanisms and brings a promising approach to solve the anode nuisance in aqueous metal batteries.