To improve the material properties and the electrochemical of ultra-high nickel (LiNixCoyMn1−x−yO2, x ≥ 9) materials for their application in LIBs, the wet chemical method followed by calcination was conducted to modify the LiNi0.96Co0.02Mn0.02O2 (LNCM9622) cathode using a conductive lithium-borate oxide (Li3BO3) coating layer. The influence of mass fractions (wt%) of Li3BO3 layer on morphology and structure properties, electrochemical performance, and Li+ diffusion coefficient of the ultra-high nickel LNCM9622 cathode was systematically investigated. The results demonstrate the Li3BO3 coating layer has not significantly altered the material phase and morphology of cathode LNCM9622; however, the I(003)/I(104) ratios and c/a parameters increased, indicating the reduction of cation mixing of Li3BO3 coated LNCM9622 cathode. The electrochemical performance test reveals that the appropriate wt% of Li3BO3 coating layer could properly stabilize the cycle and the rate discharge capacity. The LNCM9622-LBO-0.75% displayed the higher initial discharge capacity of 213.7 mAh/g and 100 cycles discharge capacity of 156.60 mAh/g, with the capacity retention of 82.20% at 1 C and 25 °C which much higher than the LNCM9622-pristine which the initial discharge capacity of 212 mAh/g, 100 cycles discharge capacity of 139.7 mAh/g, and capacity retention of 79.08%. The EIS measurement also revealed that the existence of Li3BO3 coating layer can improve the lithium-ion diffusion coefficient that seen after 100 cycles, where the optimum LNCM922-LBO-0.75% exhibits the higher diffusion coefficient of 2.74 × 10−12 cm2/s. In conclusion, this study successfully proved the use of Li3BO3 coating layer can improve both material properties and electrochemical performance of ultra-high nickel LNCM9622 cathode, with the optimum coating mass fraction was 0.75 wt% of Li3BO3.