Highly Flexible and Structurally Stable Oriented Conductive Framework for Deformation‐Tolerant Zn‐Ion Batteries

Abstract Oriented conductive frameworks with high flexibility and mechanical stability can facilitate efficient electron and ion transport in complex‐shaped power supplies, boosting the reliability and function of the next‐generation flexible electronics. Here, a multi‐direction deformable and structurally stable oriented conductive framework is presented, which is mediated by hydrogen bonding interactions of poly(3,4‐ethylenedioxythiophene)‐poly(styrenesulfonate) (PEDOT:PSS), through self‐assembly on a porous wood template. The framework exhibits excellent flexibility in three dimensions, restoring integrity and maintaining constant conductivity across diverse deformations, even after enduring 5000 bending cycles (angle: 180°) and soaking in water for 6 months. Utilizing its unique oriented structure and flexible bending capability, a flexible zinc‐iodine battery is developed, which demonstrates a high areal capacity of 3.2 mAh cm −2 and an energy density of 3.8 mWh cm −2 . Moreover, the battery is capable of high‐current charging and discharging at 20 mA cm −2 , with an impressive areal capacity of 1.9 mAh cm −2 , far superior to the existing flexible zinc‐ion batteries. It also demonstrates excellent electrochemical and mechanical stability under various deformations, including bending, twisting, and rolling, providing stable energy for a commercial toy car and a flexible screen even under hammer strikes and repeated bending. This work advances the development of high‐performance, deformation‐tolerant, flexible batteries.