LiNi1/3Mn1/3Co1/3O2 had been successfully prepared from spherical composite carbonate via a simple uniform-phase precipitation method [P. He, H. Wang, L. Qi, T. Osaka, J. Power Sources, in press] at normal pressure, using nickel, cobalt and manganese sulfate and ammonia bicarbonate as reactants. The preparation of spherical composite carbonate was significantly dependant on synthetic condition, such as the reaction temperature, feed rate, molar ratio of these reactants, etc. The optimized condition resulted in spherical composite carbonate of which the particle size distribution was uniform, as observed by scanning electronic microscopy (SEM). Calcination of the uniform composite carbonate with lithium carbonate at high temperature led to a well-ordered layer structured LiNi1/3Mn1/3Co1/3O2 as confirmed by X-ray diffraction (XRD), without obvious change in shape. Due to the homogeneity of the composite carbonate, the final product, LiNi1/3Mn1/3Co1/3O2, was also significantly uniform, i.e., the average particle size was of about 10μm in diameter and the distribution was relatively narrow. As a result, the corresponding tap density was also high, approximately 2.32gcm−3, of which the value is very near to that of commercialized LiCoO2. In the voltage range of 2.8–4.2, 2.8–4.35 and 2.8–4.5V, the discharge capacities of LiNi1/3Mn1/3Co1/3O2 electrode were 159, 168 and 179mAhg−1, respectively, with good cyclability.