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Lithium–rich cathodes have excess lithium in the transition metal layer and exhibit an extremely high specific capacity and good energy density. However, they still have some disadvantages. Here, we propose LiCoMnO4, a new nanolayer coating material with a spinel structure, to modify the surface of lithium cathode oxide (Li7/6Mn1/2Ni1/6Co1/6O2) with a layered structure. The designed cathode with nanolayer spinel coating delivers an excellent reversible capacity, outstanding rate capability, and superior cycling ability whilst exhibiting discharge capacities of 300, 275, 220, and 166 mAh g−1 at rates of 0.1 C at 2.0−4.8 V formation and 0.1, 1, and 5 C, respectively, between 2.0 and 4.6 V. The cycling ability and voltage fading at a high operational voltage of 4.9 V were also investigated, with results showing that the nanolayer spinel coating can depress the surface of the lithium cathode oxide layer, leading to phase transformation that enhances the electrochemical performance. [ABSTRACT FROM AUTHOR]