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Li||NMC811 battery, with lithium‐metal (high specific capacity and low redox potential) as anode and LiNi0.8Co0.1Mn0.1O2 (NMC811) as cathode, has been widely accepted to be a good candidate as one of the high‐energy‐density batteries. However, its cyclability needs improvement to fulfill the requirement for its future commercial use, especially under practical conditions. Electrolyte plays a key role...