Enhanced Electrochemical Stability of Sulfide Electrolytes with Surface Modification for High‐Performance LiNiO₂ Based All‐Solid‐State Lithium Batteries

at 0.2 C and 45 °C, alongside remarkable cycling stability (95% capacity retention after 200 cycles at 4.4 V). Additionally, even under an ultra-high voltage of 4.6 V, the battery can still retain 95% capacity over 140 cycles. Multimodal spectroscopic analyses confirm that the designed coating suppresses interfacial decomposition while maintaining rapid Li⁺ transport. This work establishes a scalable, cost-effective approach to interfacial engineering, unlocking the potential of LNO-based ASSLBs for high-specific energy applications.