Structural and Interfacial Engineering of Ti 3 C 2 T x Reinforced Polyacrylamide–Polyvinyl Alcohol Double‐Network Hydrogel Electrolyte for Long‐Durable Flexible Zinc‐Ion Batteries

Hydrogel electrolytes hold a prominent interest in large‐scale Zn‐based energy storage systems due to their inherent safety, low cost, and stable cycling performance. However, achieving simultaneous regulation of electrolyte structure and interface stabilization for uniform Zn 2+ deposition, dendrite suppression, and long‐term cycling stability remains an optimal challenge. Herein, the current study emphasizes the advancement of 2D‐Ti 3 C 2 T x (Ti‐MXene) incorporated polyacrylamide (PAM)–polyvinyl alcohol (PVA) double network (DN)‐based composite hydrogel electrolytes (CHGEs) for flexible zinc‐ion batteries (FZIBs). As a result, the developed PAM–PVA/Ti‐MXene (0.1 wt.%) displays excellent mechanical strength of 3.6 MPa and ionic conductivity of 22.9 mS cm −1 . In addition, the Zn//Zn symmetrical cell also exhibits a stable stripping/plating of 1000 h at 0.1 mA cm −2 as well as exceptional reversibility behavior of Zn//Cu assymetric cell with average coulombic efficiency of 99.4% for over 500 cycles. Furthermore, the fabricated Zn//V 2 O 5 battery exhibits a high discharge capacity of 178 mAh g −1 at 0.1 A g −1 and excellent capacity retention of 84% for 500 cycles with a coulombic efficiency of 100%. Overall, the present investigation of DN‐based CHGEs will provide new insights into a stable, dendrite‐free Zn anode, enabling high‐performance flexible devices and beyond.