Graphitic carbon nitride (g-CN) hybrid aerogels (GHAs) with different proportions of g-CN were prepared using g-CN, carboxymethyl cellulose, and β-cyclodextrin. GHAs have demonstrated high porosity, large specific surface area, rich three-dimensional network structure. GHAs demonstrated an excellent synergistic effect on the photocatalytic and adsorptive properties. Especially, GHA1 (the ratio of g-CN and aerogel component was 1:1) exhibited a good synergy in photodegradation and adsorption, with a Rhodamine B (Rh B) removal up to 97.99% in 90 min. In five cycling experiments, the GHA1 showed a good long-term stability. The aerogels can be easily isolated and maintains its excellent photocatalytic properties. Compared to pure g-CN, GHA1 has a stronger photocurrent, which is due to the transmission of light to the surface of the catalyst, promoted photo-generated electron-hole pairs, and inhibited recombination of electros and holes. Finally, mechanistic studies reveal that the superoxide radicals (O) are the main active groups in the photocatalytic degradation process. This work provides a useful perspective in design and fabrication of hybrid aerogel composites with an enhanced photocatalytic activity.