Structurally Engineered Soft‐Elastic Polymers as Stress‐Adaptive and Deposition‐Regulating Layers for Ultrastable and High‐Rate Zn‐Powder Anodes

Abstract To address the poor durability hindering zinc powder (Zn‐P) anodes in aqueous zinc‐ion batteries (AZIBs), soft‐elastic amino‐functionalized polymer‐modified Zn‐P anodes (P‐A2@NH 2 ) are developed inspired by a novel mechanistic understanding involving internal stress and complex ion transport. The polymer forms a dynamically swelling 3D network that facilitates internal stress mitigation and efficient Zn 2+ transport, while its amino groups modulate the solvation sheath and regulate Zn 2+ deposition. The resulting Zn‐P/P‐A2@NH 2 anode enables symmetric cells to achieve ultra‐long cycling (>8 300 h at 2.5 mA cm −2 /0.5 mAh cm −2 ) and maintains stability for 2 000 h at 25 mA cm −2 with 87.5% depth of discharge and 25 000 mAh cm −2 cumulative plating capacity. When paired with an AlVO‐H 2 O cathode, full cells deliver 314 mAh g −1 at 2 A g −1 with 91.93% capacity retention over 500 cycles at a low N/P ratio of 2.4. This work provides a fundamental and universal strategy to enhance Zn‐P anode durability, enabling ultrastable and ultrahigh‐rate AZIBs.