Cr2O3-coated LiNi1/3Co1/3Mn1/3O2 cathode materials were synthesized by a novel method. The structure and electrochemical properties of prepared cathode materials were measured using X-ray diffraction (XRD), scanning electron microscopy (SEM), charge-discharge tests, cyclic voltammetry (CV), and electrochemical impedance spectroscopy (EIS). The measured results indicate that surface coating with 1. 0 wt％ Cr2O3 does not affect the LiNi1/3Co1/3Mn1/3O2 crystal structure (α-NaFeO2) of the cathode material compared to the pristine material, the surfaces of LiNi1/3Co1/3Mn1/3O2 samples are covered with Cr2O3 well, and the LiNi1/3Co1/3Mn1/3O2 material coated with Cr2O3 has better electrochemical performance under a high cutoff voltage of 4. 5 V. Moreover, at room temperature, the initial discharging capacity of LiNi1/3Co1/3Mn1/3O2 material coated with 1. 0 wt. ％ Cr2O3 at 0. 5C reaches 169 mAh·g-1 and the capacity retention is 83. 1％ after 30 cycles, while that of the bare LiNi1/3Co1/3Mn1/3O2 is only 160. 8 mAh·g-1 and 72. 5％. Finally, the coated samples are found to display the improved electrochemical performance, which is mainly attributed to the suppression of the charge-transfer resistance at the interface between the cathode and the electrolyte.