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LiNixCoyMn1−x−yO2 (x ≥ 0.6, NCM) has attracted much attention due to its high specific capacity and energy density. However, capacity attenuation caused by Li+/Ni2+ mixing and structural instability inhibit its development and application. In order to solve these problems, we report a simple method to synthesize NCM cathodes via a one-step Ce4+-doping and CeO2-coating technique, which can reduce the degree of Li+/Ni2+ mixing and improve the structural stability. The Ce4+-doping not only effectively reduces the degree of Li+/Ni2+ mixing, but also enhances the (001) interplanar distance of NCM and improves Li+ diffusion. Furthermore, the CeO2-coating can reduce the direct contact between the NCM particles and electrolyte, which can reduce the harmful interface reaction, thus making the impedance increase more slowly. The Ce4+-doping and CeO2-coating of NCM particles led to a capacity retention of 96.3% at 1C (1C = 280 mA g−1) after 100 cycles. Therefore, the synthesis of NCM cathodes via a one-step Ce4+-doping and CeO2-coating technique is a superb way to improve the electrochemical properties of the NCM cathode in lithium-ion batteries. [ABSTRACT FROM AUTHOR]