To ameliorate the electrochemical properties and thermal stability of the Layered Li-rich and Mn-based oxides, the Li2ZrO3 nanoparticles with different contents were coated on the surface of Li1.20Mn0.54Ni0.13Co0.13O2 via using the sol–gel method. The effect of the Li2ZrO3 coating modification on the microstructure, morphology and electrochemical properties of the Li1.20Mn0.54Ni0.13Co0.13O2 cathode have been investigated by the XRD, SEM, TEM, galvanostatic discharge–charge tests and electrochemical impedance spectroscopy techniques. The results demonstrated the Li2ZrO3 coating layer not only could keep cathode away from HF and corrosive electrolyte, but also contributed to enhancing the Li+ migration speed across the interfacial regions. The 2 wt% Li2ZrO3 coated Li1.20Mn0.54Ni0.13Co0.13O2 delivered about 25.6 mAh g−1 larger than that of the pristine one at 5C high rate. In addition, the 2 wt% Li2ZrO3 coated material retained a much higher discharge capacity retention of 92.6% after 200 cycles. Whereas, the pristine cathode showed only 85.0% of the capacity retention under identical conditions. These results indicated that Li2ZrO3 coating modification could effectively enhance the electrochemical properties of Li1.20Mn0.54Ni0.13Co0.13O2.