A modified Zr-coating process was introduced to improve the electrochemical performance of Li(Ni1/3Co1/3Mn1/3)O2. The ZrO2-coating was carried out on an intermediate, (Ni1/3Co1/3Mn1/3)(OH)2, rather than on Li(Ni1/3Co1/3Mn1/3)O2. After a heat treatment process, one part of the Zr covered the surface of Li(Ni1/3Co1/3Mn1/3)O2 in the form of a Li2ZrO3 coating layer, and the other part diffused into the crystal lattice of Li(Ni1/3Co1/3Mn1/3)O2. A decreasing gradient distribution in the concentration of Zr was detected from the surface to the bulk of Li(Ni1/3Co1/3Mn1/3)O2 by X-ray photoelectron spectra (XPS). Electrochemical tests indicated that the 1% (Zr/Ni+Co+Mn) ZrO2-modified Li(Ni1/3Co1/3Mn1/3)O2 prepared by this process showed better cyclability and rate capability than bare Li(Ni1/3Co1/3Mn1/3)O2. The result can be ascribed to the special effect of Zr in ZrO2-modified Li(Ni1/3Co1/3Mn1/3)O2. The surface coating layer of Li2ZrO3 improved the cycle performance, while the incorporation of Zr in the crystal lattice of Li(Ni1/3Co1/3Mn1/3)O2 modified the rate capability by increasing the lattice parameters. Electrochemical impedance spectra (EIS) results showed that the increase of charge transfer resistance during cycling was suppressed significantly by ZrO2 modification.