Provided is a cathode composition for lithium secondary battery that includes a lithium-chromium-titanium-manganese oxide that has the formula Li[Li(1-x)/3CrxTi(2/3)yMn2(1-x-y)/3]O2 where 0≦x≦0.3, 0≦y≦0.3 and 0.1≦x+y≦0.3, and layered a-LiFeO2 structure. A method of synthesizing the lithium-chromium-titanium manganese oxide includes preparing a first mixed solution by dispersing titanium dioxide (TiO2) in a mixed solution of chrome acetate (Cr3(OH)2(CH3CO2)7) and manganese acetate ((CH3CO2)2Mn.4H2O), adding a lithium hydroxide (LiOH) solution to the first mixed solution to obtain homogeneous precipitates, forming precursor powder that has the formula Li[Li(1-x)/3CrxTi(2/3)yMn2(1-x-y)/3]O2 where 0≦x≦0.3, 0≦y≦0.3 and 0.1≦x+y≦0.3 by heating the homogeneous precipitates, and heating the precursor powder to form oxide powder having a layered structure.