Layered Li–Cr–Mn–O cathode materials related to the LiCrO2–LiMnO2–Li2MnO3 solid solution have been synthesized by the mixed-hydroxide method. The materials are characterized by X-ray diffraction (XRD) and electrochemical techniques. The XRD patterns reveal that samples are a solid solution of hexagonal and monoclinic structures. The most promising cathode material in terms of high capacity and stable cycling performance exhibits the average discharge capacity of 204mAhg−1 between 2.5 and 4.5V versus Li/Li+.