Water-Restrained Hydrogel Electrolytes with Repulsion-Driven Cationic Express Pathways for Durable Zinc-Ion Batteries

• A novel cationic hydrogel electrolyte (PAPTMA) resolves the tripartite trade-off among ionic conductivity, Zn2+ mobility, and electrochemical stability. • Cationic express pathways enable fast and selective Zn2+ transport via ionic repulsion, achieving high ionic conductivity (28.7 mS cm−1) and Zn2+ transference number (0.79). • The hydrogel exhibits exceptional cycling stability across −15 to 60 °C, with symmetric cells lasting over 6000 h at 1 mA cm−2. • Pouch cells with MnO2 cathode demonstrate remarkable operational stability and mechanical robustness over 150 cycles, highlighting practical flexible battery potential.