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Ethylene carbonate (EC) in the electrolyte is not stable in cells operated at high voltage (≥4.4V) or with Li metal anode, which greatly reduce the energy density and lifetime of the rechargeable lithium battery. Herein, an EC-free linear alkyl carbonate-based electrolyte is developed, which enables the high-voltage (≥4.4V) and low-temperature (-30°C) application of Ni-rich cathode (LiNi 0.8 Mn 0.1 Co 0.1 O 2 , NCM811). The EC-free system, consisting of LiPF 6 and LiNO 3 in ternary linear alkyl carbonates, possesses low viscosity, weakly solvated structure, and high interfacial stability with both the Ni-rich cathode and the Li metal anode to avoid continuous electrode/electrolyte side reactions and metal dissolution from the cathode. As a result, the Li||NCM811 cell delivers remarkable capacity retention of 93 ± 0.5% at the voltage of 4.4V and 88 ± 0.6% at 4.5V over 100 cycles. This study provides very encouraging perspective to develop EC-free carbonate-based electrolyte for high-voltage and low-temperature application in high-energy-density rechargeable lithium batteries., Competing Interests: The authors declare no conflict of interest., (© 2022 The Author(s).)