The demands placed on lithium-ion batteries in sectors like electric vehicles and consumer electronics are becoming increasingly stringent, necessitating features such as high energy density, long cycle life, and robust safety. Combining high-capacity silicon-based anodes (>1500 mAh g⁻¹) with high-voltage, nickel-rich ternary cathodes enables the attainment of an impressive energy density exceeding 400 Wh kg⁻¹. Nevertheless, the considerable volume expansion of silicon anodes during the charging and discharging process (approximately 400%) gives rise to challenges including structural pulverization, electrode delamination, and instability of the solid electrolyte interface. These issues lead to a continuous loss of active lithium and a swift decline in capacity. Especially under high-voltage conditions of 4.5V and across a broad temperature spectrum (ranging from 60°C to -40°C), conventional electrolytes find it difficult to establish a stable interface, presenting a significant barrier to their commercial utilization.