The spherical Li[Ni1/3Co1/3Mn1/3]O2 powders with appropriate porosity, small particle size and good particle size distribution were successfully prepared by a slurry spray drying method. The Li[Ni1/3Co1/3Mn1/3]O2 powders were characterized by XRD, SEM, ICP, BET, EIS and galvanostatic charge/discharge testing. The material calcined at 950°C had the best electrochemical performance. Its initial discharge capacity was 188.9mAhg−1 at the discharge rate of 0.2C (32mAg−1), and retained 91.4% of the capacity on going from 0.2 to 4C rate. From the EIS result, it was found that the favorable electrochemical performance of the Li[Ni1/3Co1/3Mn1/3]O2 cathode material was primarily attributed to the particular morphology formed by the spray drying process which was favorable for the charge transfer during the deintercalation and intercalation cycling.