The performance of LiNi0.8Co0.1Mn0.1O2 cathode materials has been significantly improved by Li4P2O7 surface modification. Some electrochemical tests are carried out to investigate the relevant performances of LiH2PO4 coated LiNi0.8Co0.1Mn0.1O2 , such as inductively coupled plasma test (ICP), scanning electron microscopy (SEM), X-ray diffraction (XRD), transmission electron microscopy (TEM), and X-ray photoelectron spectroscopy (XPS). The results indicate that LiNi0.8Co0.1Mn0.1O2 is clad with a layer of average thickness about 30-40 nm. And the alkalinity on the surface of the modified materials has declined dramatically after titration measurement. The effect of surface modification can be credited to the two main factors: On the one hand, the weak acidity of LiH2PO4 neutralizes the lithium residues (LiOH/Li2CO3) on the surface of LiNi0.8Co0.1Mn0.1O2 cathode materials; on the other hand, LiH2PO4 continues to decompose and react with the unneutralized lithium residues to generate a coating layer of Li4P2O7 during the annealing process, which can prevent the active materials from contacting with the electrolyte directly and act as an outstanding Li+ conductor, thus inhibiting the interface reaction and improving the cycle performance as well as the rate properties of the host materials.