The graphene-C60 hybrid has been synthesized and characterized. Its nonlinear optical property was investigated. Raman spectroscopy suggested a strong interaction between C60 and graphene. Based on UV and elemental analysis measurement, it is estimated that one C60 molecule is covalently attached for every approximately 110 carbon atoms in graphene. The nonlinear optical performance of this hybrid material was studied using the Z-scan measurement and a much enhanced nonlinear optical performance was observed compared with that of the benchmark material-C60 and graphene. This may be partially attributed to the photoinduced electron transfer mechanism between graphene and C60.