This work reports a strategy towards greener lithium-ion batteries, by employing the aqueous sodium carboxymethyl cellulose-based LiNi_0.4Co_0.2Mn_0.4O₂ (CMC/NCM) as cathode electrode. 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. As a result, CMC/NCM electrodes show good structural integrity. Additionally, these electrodes offer enhanced Li⁺ diffusion kinetics, reduced polarization, therefore, excellent high C-rate capability, and extremely stable cycling performance. In detail, CMC/NCM electrodes achieve capacity retention ratios as high as 96.4% (0.1 C), 102.9% (2 C), 111.8% (10 C), and 96.7% (at elevated temperature, i.e., 60 ^oC, 10 C) after 100 cycles. Moreover, benefiting from the features of low cost, environmentally friendliness, and easy disposability-recyclability, the water-soluble CMC is expected to be a promising binder for practical applicants in energy storage systems.