Aqueous zinc-ion batteries (AZIBs) have gained significant attentions for their inherent safety and cost-effectiveness. However, challenges, such as dendrite growth and anodic corrosion at the Zn anode, hinder their commercial viability. In this paper, an organic−inorganic coating layer (Nafion−TiO 2 ) was introduced to protect the Zn anode and electrolyte interface. Briefly, Nafion effectively shields against the corrosion from water molecules through the hydrophobic wall of −CF 3 and guided zinc deposition from the −SO 3 functional group, while TiO 2 particles with a higher Young's modulus (151 GPa vs 120 GPa from Zn metal) suppress the zinc dendrite formation. As a result, with the protection of Nafion−TiO 2, the symmetrical Zn∥Zn battery shows an improved cycle life of 1,750 h at 0.5 mA cm −2 , and the full cell based on Zn∥MnO 2 shows a long cycle life over 1,500 cycles at 1 A g −1 . Our research offers a novel approach for protecting zinc metal anodes, potentially applicable to other metal anodes such as those in lithium and sodium batteries.