Spherical Li(Ni 1/3 Co 1/3 Mn 1/3 )O 2 with a layered structure has been successfully prepared by the eutectic molten-salt method using 0.24LiCO 3 –0.76LiOH (with a melting point of 423 °C) and (Ni 1/3 Co 1/3 Mn 1/3 )(OH) 2 , where the ratio of Li/(Ni+Co+Mn) is controlled at 1:1. The tap-density of the powders obtained in this work (2.89) is remarkably higher than that of spherical Li(Ni 1/3 Co 1/3 Mn 1/3 )O 2 powders synthesized by other single lithium salts (2.40). XRD analysis shows that this material has a well-developed layered structure. Charge–discharge tests have shown that a Li(Ni 1/3 Co 1/3 Mn 1/3 )O 2 cathode prepared at 950 °C has an initial discharge capacity as high as 166. After 50 cycles, the cell showed little capacity loss, which indicated the excellent cyclic performance of the synthesized materials.