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Dendrite formation and water-triggered side reactions on the surface of Zn metal anodes severely restrict the commercial viability of aqueous zinc-ion batteries (AZIBs). In this work, we introduce erythritol (Et) as an electrolyte additive to enhance the reversibility of zinc anodes, given its cost-effectiveness, mature technology, and extensive utilization in various domains such as food, medicine, and other industries. By combining multiscale theoretical simulation and experimental characterization, it was demonstrated that Et molecules can partially replace the coordination H2O molecules to reshape the Zn2+ solvation sheath and destroy the hydrogen bond network of the aqueous electrolyte. More importantly, Et molecules tend to adsorb on the zinc anode surface, simultaneously inhibit water-triggered side reactions by isolating water and promote uniform and dense deposition by accelerating the Zn2+ diffusion and regulating the nucleation size of the Zn grain. Thanks to this synergistic mechanism, the Zn anode can achieve a cycle life of more than 3900 h at 1 mA cm−2 and an average Coulombic efficiency of 99.77%. Coupling with δ-MnO2 cathodes, the full battery delivers a high specific capacity of 228.1 mAh g−1 with a capacity retention of 76% over 1000 cycles at 1 A g−1. [ABSTRACT FROM AUTHOR]