Dual‐Functional Layer Engineering Unlocking Dendrite‐Free and High‐Performance Zinc Metal Anodes

Abstract Developing a highly stable and dendrite‐free zinc (Zn) anode is crucial for the commercial application of aqueous Zn‐ion batteries. Herein, a dual‐functional layer interface is constructed on the Zn anode surface via femtosecond laser processing strategy, and the effect of periodic micro–nano structures on accelerating the transport dynamics of Zn ions and suppressing dendrite growth is investigated. The surface oxide layer exhibits strong affinity and a low diffusion barrier for Zn ions, significantly inhibiting corrosion and side reactions. Meanwhile, the subsurface dislocation layer can suppress the deposited stress and provide uniform stress distribution to improve the strain resistance of the electrode. These integrated merits enable Zn anodes with the dual‐functional layer a high reversibility of 99.11% for 1000 cycles, and impressive cyclability for 2678 h at 2 mA cm⁻²/1 mAh cm⁻². The assembled full cell exhibits a maximum of 1300 cycles with an enhanced capacity retention rate. Notably, the large‐area pouch cell maintains stable cycling for 100 h and exhibits excellent flexibility in flexible Zn‐ion battery systems. This work highlights the crucial role of femtosecond laser‐induced periodic micro–nano structures in optimizing Zn deposition and stimulates the precise control of dislocation characteristics for achieving highly reversible Zn anodes.