Coupling Temperature‐Adaptive Solvation With Nano‐Confined Channels Enables Ultrafast Charging Batteries Spanning 140°C Window

A formidable challenge in developing high‐energy‐density lithium‐ion batteries for electric vehicles and aviation lies in enabling ultra‐fast charging and wide‐temperature operation, originating from trade‐offs in electrolyte design. The electrolyte must reconcile high ionic conductivity, minimal desolvation penalties, and low melting points, while deriving a robust, anion‐rich inorganic interphase to guarantee superior interfacial kinetics and thermal safety. Herein, this work surpasses the conventional dichotomy of isolated electrode engineering or electrolyte formulation, proposing a holistic strategy that synergises a dual‐doped high‐rate anode with a temperature‐responsive, weakly solvating electrolyte. This design engineers an anion‐rich environment across the inner and outer Helmholtz planes, facilitating Li + desolvation kinetics at sub‐zero temperatures while suppressing parasitic reactions under high‐temperature conditions. Validated across both coin and pouch cells, the devices exhibit outstanding durability, preserving 99% of nominal capacity at 1 C even at an ultralow temperature of −60°C. Conversely, under aggressive 80°C conditions, they sustain 85% capacity retention after 500 cycles at a high rate of 10 C. These metrics correspond to unparalleled cycling stability and rate capability across a broad 140°C operating window. This work presents a pragmatic solution for energy storage applications in extreme climates.