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A mixed cathode material between Li2MnO3 and Li[Mn1/3Ni1/3Co1/3]O2 for high capacity lithium secondary batteries was introduced in this study. It was prepared using the sucrose combustion process because this is a simple process. The oxidation states of Mn, Co and Ni ions in the pristine Li[Li(1−x)/3Mn(2−x)/3Nix/3Cox/3]O2 compounds were confirmed to be tetravalent, trivalent and divalent, respectively, via XANES measurements. Electrochemical charge/discharge studies showed that the highest first discharge capacity of 224 mAh/g was obtained in composition of x = 0.5 at a 0.2 C rate. The oxidation state of the Co and Ni ions in the Li[Li1/6Mn1/2Ni1/6Co1/6]O2 changed to higher oxidation states, but that of the Mn ions did not change.