The covalent attachment of poly(2-hydroxyethyl methacrylate) on ZnO nanoparticles (NPs) has been achieved by ARGET ATRP. The polymer chains were grown from the surface of ATRP-initiator modified ZnO NPs with a copper (II) catalyst under activation of zerovalent copper as a reducing agent. FT-IR, FE-SEM, TEM and TGA were employed for the characterization of the nanocomposites. GPC was used to determine the molecular weight and PDI of the cleaved polymer. The covalent attachment of polymer chains onto the surface of ZnO NPs was sufficiently confirmed by FT-IR. In addition, the formation of the polymer encapsulating ZnO cores was demonstrated from TEM and SEM images. It was found that the growing of polymer brushes from the ZnO surface could be induced even though the catalyst amount was reduced to 10 ppm without loss of inherent control manner. This report contributed to demonstrate the versatility and feasibility of ATRP-based surface-initiated polymerization for the preparation of inorganic/polymer nanocomposites.