This work reports the performance of LiNi0.4Co0.2Mn0.4O2 electrodes employing sodium carboxymethyl cellulose as the binder (CMC/NCM). Compared with conventional organic PVDF-based electrodes, the CMC/NCM electrodes display very uniform distribution of NCM and carbon particles together with strong adhesion among the particles and with the current collector, leading to significantly mitigated crack formation and delamination of the electrode upon repeated delithiation/lithiation processes. Additionally, these electrodes offer enhanced Li+ diffusion kinetics, reduced polarization, therefore, excellent high C-rate capability, and extremely stable cycling performance even at elevated temperature (60 °C). Benefiting from the features of low cost, environmentally friendliness, and easy disposability-recyclability, the water-soluble CMC is a promising binder for practical application in energy storage systems.