The layered compound Li[Ni1/3Co1/3Mn1/3]O2 was synthesized using a combination of the co-precipitation and the solid phase reaction method. The samples were characterized by X-ray diffraction, scanning electron microscopy, cyclic voltammetry and galvanostatic charge/discharge profile measurements. The results showed that the layer-structured compound Li[Ni1/3Co1/3Mn1/3]O2 was successfully formed. The morphology of the powder featured a hierarchical micron-scale spherical shape which was composed of agglomerated nanoparticles. The temperature of the synthesis affected the electrochemical properties of the resulting compound. The samples synthesized at 850 °C showed a higher initial specific capacity (176 mAh/g), and a higher reversible discharge capacity (157 mAh/g), as well as better cycling stability at the current density of 20 mA/g, compared to the samples synthesized at other temperatures. When the current densities for charge/discharge were increased, the sample synthesized at 850 °C still showed the best electrochemical performance among all the samples. The Li[Ni1/3Co1/3Mn1/3]O2 synthesized at 850 °C is a promising cathode material for lithium ion battery application.