The development of high-performance adsorbents for water purification is of utmost importance. Herein, we report the construction of a 3D graphene hybrid aerogel integrated with hollow carbon spheres via a two-step synthetic strategy. The structure and morphology of the hollow carbon spheres/graphene aerogels (HCSs/GAs) were characterized using BET, XRD, FTIR, Raman, XPS, and FESEM. The HCSs/GAs monoliths with high surface area (356.1 m(2) g(-1)) were utilized as an effective adsorbent for the removal of methyl orange (MO) and rhodamine B (RhB) dyes, organic solvents and oils from aqueous solutions. The HCSs/GAs demonstrated remarkably broad-spectrum adsorption performance with a high capacity for MO (344.1 mg g(-1)) and RhB (441.5 mg g(-1)), and up to 58-108 times its own weight for oils/organic solvents. Furthermore, the HCSs/GAs showed a rapid adsorbing ratio and superior recycling stability for oils/organic solvents. The adsorption kinetics of the HCSs/GAs were investigated and were well-fitted by the pseudo-second-order kinetics model. The high performance of the HCSs/GAs is related to its interconnected 3D hierarchical porous framework, high surface area and large pore volume. Therefore, the HCSs/GAs are believed to be a promising adsorbent for wastewater treatment.