LAUSR

Zinc (Zn) metal anode has been widely evaluated in aqueous Zn batteries. Nevertheless, the dendrite formation issue and consecutive side reactions severely impede the practical applications of Zn metal at high current densities. Herein, it is reported that engineering the gel electrolyte with multifunctional charged groups by incorporating a zwitterionic gel poly(3‐(1‐vinyl‐3‐imidazolio) propanesulfonate) (PVIPS) can effectively address the abovementioned issues. The charged groups of sulfonate and imidazole in the gel electrolyte can texture the Zn2+ nucleation and deposition plane to (002), which possesses a high activation energy to resist side reactions and induce uniform growth of Zn metal for a dendrite‐free structure. In addition, the Zn2+ solvation structure can be manipulated by the charged groups to further eliminate side reactions for high rate performance Zn batteries. Consequently, the polyzwitterionic gel electrolyte enables a stable cycling with a cumulative capacity of 3000 mA h cm−2 at high density of 7.5 mA cm−2 for the symmetrical Zn battery, and a long‐term cycling life for more than 1000 cycles at 5 C of Zn/MnO2 full battery. It is envisioned that the design of the gel electrolyte will provide promising feasibility on safe, flexible, and wearable energy storage devices.