With the fast development of modern industry, heavy metal contaminant became more severe. How to remove heavy metal ions in water in a green and efficient way is a prominent problem in current environmental protection. The adsorption of cellulose aerogel as a novel heavy metal removal technology has many advantages, including abundant resources, environmental friendly, high specific surface, high porosities and without second pollution, which means it has a wide application prospect. Here, we reported a self-assembly and covalent crosslinking strategy to prepare elastic and porous cellulose aerogels using PVA and graphene and cellulose as precursor. The resulting cellulose aerogel had a low density of 12.31 mg cm−3and excellent mechanical properties, which can recover to its initial form at 80% compressive strain. Meanwhile, the cellulose aerogel had strong adsorption capacity of Cu2+(80.12 mg g−1), Cd2+(102.23 mg g−1), Cr3+(123.02 mg g−1), Co2+(62.38 mg g−1), Zn2+(69.55 mg g−1), and Pb2+(57.16 mg g−1). In addition, the adsorption mechanism of the cellulose aerogel was investigated using adsorption kinetics and adsorption isotherm, and the conclusion was that the adsorption process was mainly controlled by chemisorption mechanism. Therefore, cellulose aerogel, as a kind of green adsorption material, has a very high application potential in future water treatment applications.