LiNi1/3Mn1/3Co1/3O2 was prepared by both the spray dry method and the metal acetate decomposition method. The influences of synthesis method on the electrochemical behaviors of LiNi1/3Mn1/3Co1/3O2 were also characterized. The difference in preparation method results in the difference in compound color, morphology (shape, particle size and specific surface area) and the electrochemical characteristics, such as the shape of first charge curve, reversible capacity and the rate capability. A sample prepared by the spray dry method exhibits an absence of 4.5V plateau, a higher capacity retention and better rate capability than those prepared by the metal acetate decomposition method. The reversible capacity after 35 cycles is 166mAhg−1 at 50°C when a cell is cycled at a current density of 0.2mAcm−2 in 3–4.5V. The operation temperature has little influence on the rate capability of the sample prepared by the spray dry method while pronounced in the case of those samples prepared by the metal acetate decomposition method.