Carboxymethyl cellulose (CMC), a green and low-cost binder, is used to make lithium-ion battery composite electrodes containing the high voltage cathode material Li2MnO3–LiMO2. This combination of materials results in a homogeneous electrode, which is proved by electron microscopy. The results of the electrochemical investigation indicate that CMC operates well at very high voltages (4.8V). Compared to the PVDF binder, the CMC-based electrode shows an improved cycling stability as well as a very promising rate capability.