• Developed an entropy-enhanced AgCuZnSnS4 loaded graphite felt (ACZTS/GF) electrode via in-situ solvothermal synthesis, achieving high energy efficiency of 88.5% at 20 mA·cm−2 and a maximum power density of 119.8 mW·cm−2 in polysulfide/iodide flow batteries.
• Introduced a targeted orbital hybridization-optimized electron density strategy that enhances catalytic activity by modulating electronic density of states and promoting synergistic effects among multinary components.
• Demonstrated that multicomponent sulfides with high configurational entropy significantly improve interfacial charge transfer kinetics and bulk conductivity, overcoming sluggish iodide redox kinetics.
• Achieved excellent long-term cycling stability with only 5% degradation, highlighting the practical viability of the engineered electrode for large-scale energy storage applications.