Layered Li(Ni2/3Mn1/3)O-2 compounds are prepared by freeze-drying, mixed carbonate and molten salt methods at high temperature. The phases are characterized by X-ray diffraction, Rietveld refinement, and other methods. Electrochemical properties are studied versus Li-metal by charge-discharge cycling and cyclic voltammetry (CV). The compound prepared by the carbonate route shows a stable capacity of 145 (+/- 3) mAh g(-1) up to 100 cycles in the range 2.5-4.3 V at 22 mA g(-1). In the range 2.5-4.4 V at 22 mA g(-1), the compound prepared by molten salt method has a stable capacity of 135 (+/- 3) mAh g(-1) up to 50 cycles and retains 96% of this value after 100 cycles. Capacity-fading is observed in all the compounds when cycled in the range 2.5-4.5 V All the compounds display a clear redox process at 3.65-4.0 V that corresponds to the Ni2+/3+-Ni3+/4+ couple. (c) 2006 Published by Elsevier B.V.