Hydrophobic polymer brushes have been grafted from graphene oxide nanosheets (GO) via the facile surface-initiated redox radical polymerization of tert-butyl acrylate (tBA) from the GO with cerium ammonium nitrate (CAN) as an oxidant. After the hydrophobic surface modification, the poly(tert-butyl acrylate) (PtBA)-grafted graphene oxide nanosheets (GO-PtBA) could still be dispersed in water because of the remaining oxygencontaining groups but deposited within 40 min. The feature makes it an easily separable adsorbent for environmental pollutants. For example, tetrabromobisphenol A (TBBPA) could be removed from aqueous solution via hydrogen bonds (between hydroxyl groups of TBBPA and hydroxyl and carboxyl groups of GO) and pi-pi interactions (between the benzene ring of TBBPA and GO), with an adsorption capacity of 22.2 mg at pH 7.0. The TBBPA-adsorbed GO-PtI3A could be deposited completely within 30 min, and the adsorbed TBBPA could be easily desorbed with ethanol, demonstrating its good recyclability.