• • Ultrathin PDMS interphase (~5 nm) achieves 2.28-fold enhancement in Zn2+ transference number, enabling rapid ion transport and low polarization, critical for high-rate and high-energy-density batteries.
• • The PDMS-modified anode delivers 99.9% Coulombic efficiency over 3500 cycles, indicating exceptional reversibility and minimal side reactions, essential for long-cycle-life energy storage.
• • Symmetrical cells operate stably for 880 hours at 60% depth of discharge, demonstrating high Zn utilization and dendrite suppression, which is vital for practical high-energy-density AZIBs.
• • Full cells with lean Zn (N/P ratio 5.7) sustain 2500 cycles, and pouch cells with high cathode loading (~7.2 mg cm−2) achieve 1400 cycles with only 0.01% decay rate, proving scalability and commercial viability.