Dynamic Solvation Perturbation Enables Fast‐Exchange Interfacial Water Regulation for Stable Aqueous Zinc Batteries

ABSTRACT Interfacial instability remains the major barrier for practical aqueous zinc batteries. Conventional electrolyte design mainly focuses on reducing water coordination number in the Zn 2+ solvation shell. However, this static criterion often neglects ligand‐exchange kinetics and can still leave highly reactive water at the interface. Herein, we propose a dynamic solvation perturbation (DSP) strategy to regulate Zn 2+ solvation through transient solvent coordination. Descriptor‐guided screening identifies methyl acetate (MA) as an optimal modulator with balanced Zn 2+ coordination and water regulation. MA forms a fast‐exchange mixed solvation sheath, shortens water residence time, and passivates residual water via dynamic solvation‐shell rearrangement. Additionally, MA exhibits facet‐selective adsorption on Zn anode, which suppresses direct water attack and promotes uniform Zn nucleation. As a result, the DSP‐regulated electrolyte enables the Zn anode to achieve long‑term cycling life over 8000 h at 1 mA cm −2 and 1 mAh cm −2 . Remarkably, stable cycling is maintained for more than 2000 h at 32% DOD and more than 1000 h at 80% DOD. In addition, the Zn||V 2 O 5 pouch‐cell with the MA‐containing electrolyte exhibits approximately 80% capacity retention over 300 cycles at 0.1 A g −1 , highlighting its potential for practical applications.