Utilising a general protocol for making surface-imprinted core-shell microparticles via a RAFT-mediated approach, we developed a Cu(II) imprinted polymer with a novel magnetic nanosphere, g-Fe 2 O 3 @meso-SiO 2 , as support. Attributed to the controlled/living polymerization mechanism of the RAFT polymerization process, the Cu(II) imprinted polymer prepared by RAFT polymerization (IIP-RAFT) presented a more well-defined morphology, more mono-dispersed properties, and much higher magnetic responsiveness, compared to the Cu(II) imprinted polymer prepared by traditional free-radical polymerization (IIP-TP). Moreover, in the static saturation binding experiments, a higher binding capacity of IIP-RAFT (210 mg g À1 ) than IIP-TP (145 mg g À1 ) was also found. Afterwards, a series of adsorption experiments were carried out to systematically evaluate the adsorption performance of the as-prepared IIP-RAFT. And the results showed that IIP-RAFT exhibited excellent selectivity, good reusability and desirable dynamic adsorption behavior, and could be an ideal candidate for SPE sorbents for the removal of Cu(II) in real wastewater. † Electronic supplementary information (ESI) available. See