Zr‐modified LiNi1/3Co1/3Mn1/3−xZrxO2 samples were prepared through a rheological‐phase method. The results indicate that there is only partial Zr doping into the bulk phase of the LiNi1/3Co1/3Mn1/3O2 particles, whereas the rest of the Zr remained on the surface to form a Li2ZrO3 coating layer during the Zr‐modification process. The Zr‐modified LiNi1/3Co1/3Mn1/3−xZrxO2 samples show lower discharge specific capacities at low rates, however, which exhibit clearly improved rate capabilities than that of pristine LiNi1/3Co1/3Mn1/3O2. Among the Zr‐modified LiNi1/3Co1/3Mn1/3−xZrxO2 samples, LiNi1/3Co1/3Mn1/3−0.01Zr0.01O2 (x=0.01) shows the best rate capability, which exhibts158, 142, and 132 mAh g−1 at 1.0, 2.0, and 3.0 C, respectively. The related results indicate that the doped Zr in pristine LiNi1/3Co1/3Mn1/3O2 could improve the structure stability and the formation of an inactive Li2ZrO3 coating layer which could suppress the interfacial side reaction of LiNi1/3Co1/3Mn1/3O2.