Recently, there have been many reports on efforts to improve the rate capability and discharge capacity of lithium secondary batteries in order to facilitate their use for hybrid electric vehicles and electric power tools. In the present work, we present a ZrO2-coated Li[Li1/6Mn1/2Co1/6Ni1/6]O2. The bare Li[Li1/6Mn1/2Co1/6Ni1/6]O2 shows a high initial discharge capacity of 224 mAh g−1 at a 0.2 C rate. Owing to the stability of ZrO2, it was possible to enhance the rate capability and cyclability. After 1 wt% ZrO2 coating, the ZrO2-coated Li[Li1/6Mn1/2Co1/6Ni1/6]O2 showed a high discharge capacity of 115 mAh g−1 after 50 cycles under a 6 C rate, whereas the bare Li[Li1/6Mn1/2Co1/6Ni1/6]O2 showed a discharge capacity of only 40 mAh g−1 and very poor cyclability under the same conditions. Based on results of XRD and EIS measurements, it was found that the ZrO2 suppressed impedance growth at the interface between the electrodes and electrolyte and prevented collapse of the layered hexagonal structure.