Lithium-manganese-cobalt oxide, Li(Lix/3Mn2x/3Co1-x)O-2 (0 less than or equal to x less than or equal to 1) was prepared as a solid solution between the two kinds of layer structured end members, LiCoO2 and Li2MnO3. Excess lithium carbonate or lithium hydroxide should be added to the mixture on calcination at 900 - 1000 degrees C to obtain the solid solutions. The resulting layer structured solid solutions can be used as a cathode material for secondary lithium batteries.