Three-dimensional porous graphene-based aerogels have become one of the most promising adsorbent materials for water pollution because of their unique structure and superhigh adsorption properties. However, most pore structures of graphene-based aerogels only have affinity for certain types of pollutants. This restricts the industrial application of graphene-based aerogels to a certain extent. In this study, superelastic graphene/carboxymethyl cellulose composite aerogels (SGA/CMC) were prepared under ambient pressure. And the effects of reducing agent dosage, prereduction time and pH value on the formation of aerogel were investigated. FTIR, XRD, XPS, Raman, SEM and microcomputer-controlled electronic universal testing machine were used to characterize the structure, stress-strain and micromorphology of SGA/CMC. The results show that SGA/CMC can not only adsorb the pure organic compound, but also the dye in water. The static adsorption rate of cyclohexane on water surface is 13.15 g g(-1) s(-1), and the removal rate of methylene blue in water can reach 99.7%. In addition, SGA/CMC shows high elasticity and fatigue resistance. After 500 cycles of cyclic compression at 80% strain, it can still recover to about 95% of the original height.