Multiscale Interface Engineering From Atomic Heterojunction to Macroscopic Array for Stable Zinc Metal Anode

ABSTRACT Aqueous zinc‐ion batteries hold great promise for sustainable energy storage, yet uncontrolled Zn dendrite formation critically limits their cyclability. To address this issue, a type‐II band alignment‐driven bidirectional heterojunction array is engineered as a multifunctional interface layer for the Zn anode. This multiscale vertical array architecture simultaneously regulates electric field distribution, homogenizes Zn 2+ ion flux, and mitigates electrodeposition stress, thereby promoting uniform and reversible Zn plating/stripping. As a result, the modified anode achieves a high depth of discharge of 85.5% and sustains stable cycling for over 350 h at 5 mA cm −2 /5 mAh cm −2 . When paired with an iodine‐based cathode, the full cell retains 184.4 mAh g −1 after 10 000 cycles. The use of readily available materials, combined with a scalable fabrication approach and rationally designed multiscale interface, offers a practical and inspiring strategy toward high‐performance zinc‐based energy storage systems.