Layered Li[Ni 0.5−x Mn 0.5−x Zr 2x ]O 2 (x=0, 0.025) have been prepared by the mixed hydroxide and molten-salt synthesis method. The individual particles of synthesized materials have a sub-microsize range of 200–500nm, and LiNi 0.475 Mn 0.475 Zr 0.05 O 2 has a rougher surface than that of LiNi 0.5 Mn 0.5 O 2 . The Li/Li[Ni 0.5−x Mn 0.5−x Zr 2x ]O 2 (x=0, 0.025) electrodes were cycled between 4.5 and 2.0V at a current density of 15mA/g, the discharge capacity of both cells increased during the first ten cycles. The discharge capacity of the Li/LiNi 0.475 Mn 0.475 Zr 0.05 O 2 cell increased from 150 to 220mAh/g, which is 50mAh/g larger than that of the Li/LiNi 0.5 Mn 0.5 O 2 cell. We found that the oxidation of oxygen and the Mn 3+ ion concerned this phenomenon from the cyclic voltammetry (CV). Thermal stability of the charged Li[Ni 0.5−x Mn 0.5−x Zr 2x ]O 2 (x=0, 0.025) cathode was improved by Zr doping.