AbstractRechargeable aqueous Zn‐ion batteries (ZIBs) are considered as a new energy storage device for wearable electronic equipment. Nowadays, dendrite growth and uneven deposition of zinc have been the principal problems to suppress the development of high‐performance wearable zinc‐ion batteries. Herein, a perovskite material of LaAlO3 nanoparticle has been applied for interface engineering and zinc anode protection. By adjusting transport channels and accelerating the Zn2+ diffusion, the hydrogen evolution reaction potential is improved, and electric field distribution on the Zn electrode surface is regulated to navigate the fast and uniform deposition of Zn2+. As a proof of demonstration, the assembled LAO@Zn||MnO2 batteries can display the highest capacity of up to 140 mAh g−1 without noticeable decay even after 1000 cycles. Moreover, a motor‐driven fan and electronic wristwatch powered by wearable ZIBs can demonstrate the practical feasibility of LAO@Zn||MnO2 in wearable electronic equipment.