Poor cycling stability and rate capability are two key issues needing to be solved for Li‐ and Mn‐rich oxide cathode material for lithium‐ion batteries (LIBs). Herein, a novel perovskite electron–ion mixed conductor Nd0.6Sr0.4CoO3 (NSCO) is used as the coating layer on Li1.2Ni0.13Co0.13Mn0.54O2 (LNCMO) to simultaneously enhance its cycling stability and rate capability. By coating 3 wt% NSCO, LNCMO–3NSCO exhibits an optimal cycling performance with a capacity retention of 99% at 0.1C (1C = 200 mA g−1) after 60 cycles, 91% at 1C after 300 cycles, and 54% at 20C after 1000 cycles, much better than 78%, 63%, and 3% of LNCMO, respectively. Even at a high charge and discharge rate of 50C, LNCMO–3NSCO exhibits a discharge capacity of 53 mAh g−1 and a mid‐point discharge voltage of 2.88 V, much higher than those of LNCMO (24 mA h g−1 and 2.40 V, respectively). Benefiting from the high electronic conductivity (1.46 S cm−1) and ionic conductivity (1.48 × 10−7 S cm−1), NSCO coating not only suppresses transition metals dissolution and structure transformation, but also significantly enhances electronic conductivity and Li+ diffusion coefficient of LNCMO by an order of magnitude.