A highly efficient adsorbent for methylene blue (MB) adsorption was developed by combination of carboxymethyl cellulose (CMC) and graphene oxide (GO) via a simple one-step hydrothermal method. The as-synthesized CMC/GO composite aerogel has a mesoporous structure with an average pore diameter of 30 nm and a high specific surface area of 800.85 m²·g⁻¹. Moreover, the CMC/GO composite aerogel demonstrates a significant selectivity for the dye adsorption, especially for MB, where its adsorption capacity can reach 244.99 mg·g⁻¹ with an excellent recyclability for more than nine times. Thus, the prepared CMC/GO composite aerogel would be an effective adsorbent for dyes adsorption, owing to the merits of high efficiency, reusability, and eco-friendliness.