Many scientific efforts have been undertaken toward reducing the Co content in LiMn1/3Ni1/3Co1/3O2 cathode materials for thin-film batteries. In this study, we present cathodes with a wide range of Li(Ni, Mn, Co)O2 compositions to determine the material with the best electrochemical performance by changing the ratio of Ni to Mn at a fixed 0.1 at.% of Co by the continuous composition spread sputtering method. The cathode composition measurements by Rutherford backscattering spectroscopy show that the best electrochemical performance is obtained for a composition of Ni:Mn:Co = 19:71:10. The reasons for this improved electrochemical performance are further investigated by X-ray diffraction, electrochemical impedance spectroscopy, Fourier-transform infrared spectroscopy, and X-ray absorption near edge spectroscopy.