A molecularly imprinted polymer-graphene oxide hybrid material was synthesized by atom transfer radical polymerization. The formation of this hybrid material was verified by Raman spectroscopy and energy dispersive spectrum. Transmission electron microscopy and atomic force microscopy showed that the average thickness of the imprinted polymer grafted on the surface of graphene oxide is about 10.957 nm. Moreover, the hybrids bind the original template 2,4-dichlorophenol with an appreciable selectivity over structurally related compounds. In addition, the method could lead to further development of graphene-based nanoelectronics.