This study addresses the significant challenge of cathode dissolution in aqueous zinc-ion batteries (AZIBs), particularly at low current densities (<1C), which limits their practical stability to only 50–100 cycles. By leveraging density functional theory (DFT) calculations, the researchers developed an artificial interphase that combines hydrophobicity and the restriction of outward penetration of dissolved vanadium cations, effectively shifting the reaction equilibrium and suppressing vanadium dissolution. This approach results in one of the best cycling stabilities to date, with no noticeable capacity fading after more than 200 cycles (≈720 h) at 200 mA g⁻¹ (0.47C). The study provides a universal design strategy for highly stable AZIBs, accelerating their industrialization. The findings highlight the importance of managing the interaction between water and the electrode material to prevent dissolution, and the proposed strategy can be applied to various VOx cathode materials, demonstrating its broad applicability.This study addresses the significant challenge of cathode dissolution in aqueous zinc-ion batteries (AZIBs), particularly at low current densities (<1C), which limits their practical stability to only 50–100 cycles. By leveraging density functional theory (DFT) calculations, the researchers developed an artificial interphase that combines hydrophobicity and the restriction of outward penetration of dissolved vanadium cations, effectively shifting the reaction equilibrium and suppressing vanadium dissolution. This approach results in one of the best cycling stabilities to date, with no noticeable capacity fading after more than 200 cycles (≈720 h) at 200 mA g⁻¹ (0.47C). The study provides a universal design strategy for highly stable AZIBs, accelerating their industrialization. The findings highlight the importance of managing the interaction between water and the electrode material to prevent dissolution, and the proposed strategy can be applied to various VOx cathode materials, demonstrating its broad applicability.