Graphene based aerogel has become one of the most likely functional adsorption materials that is applicable to purify various contaminated water sources, such as dye wastewater, because of its high porosity, structural stability, large specific surface area, and high adsorption capacity. In this study, chitosan and graphene oxide were first selected as the matrix to prepare the composite hydrogel through the hydrothermal method, which was further frozen and dried to obtain the target aerogel. The microscopic structures and adsorption capacity of the composite aerogel were then characterized by Fourier transform infrared spectroscopy (FT-IR), scanning electron microscopy (SEM), X-ray powder diffraction (XRD) and N2 (nitrogen) physical adsorption and desorption tests. The results show that the specific surface area of the composite aerogel was reached at 297.431 m2/g, which is higher than that of graphene oxide aerogel and chitosan aerogel. The aperture was reduced to about 3 nm. The adsorption rate of the composite aerogel for the methyl orange solution was as high as 97.2% at pH = 1, and the adsorption capacity was 48.6 mg/g. The adsorption process of the composite aerogel satisfies the Langmuir equation and can be described by the second-order adsorption kinetics. In addition, it is worth noting that this composite aerogel can provide a striking adsorption characteristic on methyl orange due to the combining effects from massive amino groups on chitosan and the structural conjugation of graphene oxide.