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Solid electrolyte interphase (SEI) formation and H2O activity reduction in Water‐in‐Salt electrolytes (WiSE) with an enlarged stability window of 3.0 V have provided the feasibility of the high‐energy‐density aqueous Li‐ion batteries. Here, we extend the cathodic potential of WiSE by rationally controlling intermolecular interaction and interphase chemistry with the introduction of trimethyl phosphate (TMP) into WiSE. The TMP not merely limits the H2O activity via the strong interaction between TMP and H2O but also contributes to the formation of reinforced SEI involving phosphate and LiF by manipulating the Li+ solvation structure. Thus, water‐tolerance LiMn2O4 (LMO)||Li4Ti5O12 (LTO) full cell with a P/N ratio of 1.14 can be assembled and achieve a long cycling life of 1000 times with high coulombic efficiency of >99.9 %. This work provides a promising insight into the cost‐effective practical manufacture of LMO||LTO cells without rigorous moisture‐free requirements. [ABSTRACT FROM AUTHOR]

LiNixCoyMnzO2 (x+y+z=1)||graphite lithium‐ion battery (LIB) chemistry promises practical applications. However, its low‐temperature (≤ −20 °C) performance is poor because the increased resistance encountered by Li+ transport in and across the bulk electrolytes and the electrolyte/electrode interphases induces capacity loss and battery failures. Though tremendous efforts have been made, there is still no effective way to reduce the charge transfer resistance (Rct) which dominates low‐temperature LIBs performance. Herein, we propose a strategy of using low‐polarity‐solvent electrolytes which have weak interactions between the solvents and the Li+ to reduce Rct, achieving facile Li+ transport at sub‐zero temperatures. The exemplary electrolyte enables LiNi0.8Mn0.1Co0.1O2||graphite cells to deliver a capacity of ≈113 mAh g−1 (98 % full‐cell capacity) at 25 °C and to remain 82 % of their room‐temperature capacity at −20 °C without lithium plating at 1/3C. They also retain 84 % of their capacity at −30 °C and 78 % of their capacity at −40 °C and show stable cycling at 50 °C. [ABSTRACT FROM AUTHOR]