The unstable zinc anode/electrolyte interface induced by corrosion, interfacial water splitting reaction, and dendrite growth seriously degrades the performances of metal Zn anode in aqueous electrolyte. Herein, the nucleation and growth of zinc hydroxide sulfate (ZHS), an interfacial by-product, has been tailored by Tween 80 in the electrolyte, which thereby assists in in-situ forming a dense solid electrolyte interphase (SEI) with small-sized ZHS and evenly distributed Tween 80. This SEI has high corrosion resistance and uniform distribution of zinc ions, which not only contributes to blocking the interfacial side reactions but also induces stable and calm zinc plating/stripping. Consequently, the modified electrolyte can confer the assembled Zn||Zn symmetric cell with a stable operation life over 1500 h at 1 mA·cm⁻² and 1 mAh·cm⁻² as well as the practical Zn||NH₄V₄O₁₀ full battery with a high-rate capacity of 120 mAh·g⁻¹ at the current density of 5 A·g⁻¹. This work provides a way for regulating and reusing interfacial by-products, and a new sight on stabilization electrodes/electrolyte interfaces.