Immobilizing Zwitterionic Molecular Brush in Functional Organic Interfacial Layers for Ultra-Stable Zn-Ion Batteries

• An organic-assisted solid electrolyte interface pre-construction creates a functional organic interfacial layer (OIL-IPS@Zn) with aligned zwitterionic structures, suppressing side reactions and enhancing Zn2+ transport. • OIL-IPS@Zn shows superior electrolyte affinity, enabling symmetric cells to operate stably for 3500 h at 1 mA cm−2/1 mAh cm−2 and 3200 h at 50 mA cm−2/10 mAh cm−2. • With 99.90% Zn plating/stripping efficiency, full cells paired with H2V3O8 cathodes achieve over 7000 cycles. • Density functional theory calculations and experiments confirm that immobilized organic propane sulfonate lowers energy barriers and increases Zn2+ transport kinetics.