Although the LiNi 0.8 Co 0.1 Mn 0.1 O 2 (NCM811) material has a high energy density, poor cycling stability and inferior rate capability restrict its commercialization. Surface modification is an effective strategy to improve the electrochemical performance of the NCM811 cathode. Herein, terephthalic acid (TPA) is introduced as a surface-modifying material to functionalize the NCM811 because of its multiple advantages, such as reducing the surface alkalinity and activity of the NCM811, providing a vast electronic channel and Li + diffusion pathway, and inhibiting irreversible phase transition. As proof, the asoptimized 1TPA@NCM811 cathode delivers an enhanced initial discharge specific capacity over 216 mA h g −1 , an optimized rate capability up to 5C, and a reduced irreversible capacity loss after 100 charge−discharge cycling times at 1C. Therefore, this work provides a potential pathway to effectively boost the electrochemical performance of the NCM811 cathode for its practical application.