Aqueous Zn-ion batteries (AZIBs) deliver eminent potential as next-generation energy storage systems due to the attractive merits of inherent safety and low cost. However, uncurbed dendrite growth and non-negligible water-induced side reactions could be fatal to the stability of Zn anode and commercial development of AZIBs. Herein, we construct a bifunctional zincophilic-hydrophobic interfacial layer (STA-ZnO layer) for attaining a stable Zn anode. The exposed hydrophobic alkyl chain can repel H2O to reach the Zn foil surface, efficaciously alleviating the HER and corrosion side reaction. Meanwhile, the zincophilic ZnO ensures that STA-ZnO@Zn anode accelerates Zn2+ deposition and constrains the growth of Zn dendrite. Benefitting from these advantages, symmetric cells based on STA-ZnO@Zn anode deliver long-term cycling stability over 4900 h and 4000 h at 1 mA cm−2 and 5 mA cm−2 for 1 mAh cm−2, respectively. Encouragingly, STA-ZnO@Zn anode also exhibits a high average CE of 99.81% (2000 cycles). This work develops a feasible strategy to protect Zn anode for achieving practical application of AZIBs.