Organic Radical-Boosted Ionic Conductivity in Redox Polymer Electrolyte for Advanced Fiber-Shaped Energy Storage Devices

• Developed a versatile HT-based redox polymer electrolyte with exceptional ionic conductivity (73.5 mS cm−1) through self-exchange reaction-based ion hopping mechanism and enhanced polymer chain mobility. • Achieved superior electrochemical performance (25.4 Wh kg−1 at 25,000 W kg−1) in fiber-shaped energy storage devices without additional active materials by utilizing HT as both ionic conductor and redox-active species. • Demonstrated excellent mechanical stability with 91.2% capacitance retention after 8,000 bending cycles, highlighting suitability for wearable applications. • Provided a promising pathway for next-generation flexible energy storage devices by addressing the low ionic conductivity challenge of polymer electrolytes.