CoFe2O4-reduced graphene oxide nanocomposites (CFG) have been successfully synthesized via one-step solvothermal method. The prepared CFG are characterized by X-ray diffraction, Raman spectroscopy, Fourier transform infrared spectroscopy, field emission scanning electron microscopy (FESEM), vibrating sample magnetometer and so on. The FESEM results show that CFG have uniform core-shell structure with an average diameter of about 75 nm and the thickness of the outer graphene shell is about 15–20 nm. The mass ratio of CoFe2O4 to graphene oxide is a key factor affecting the formation of core-shell hybrids. CFG display much higher adsorption capacity for anionic dyes than cationic dyes owing to the favorable electrostatic interaction. The adsorption capacity for methyl orange is observed as high as 263 mg g–1 at 298 K, and the adsorption isotherms follow the Langmuir model. Furthermore, the specific saturation magnetization (Ms) of CFG is 32.8 emu g–1, and the as-synthesized nanocomposites can be easily separated by external magnetic field after adsorption. The results suggest that CFG have great potential for the practical industrial wastewater treatment.