A sub-micron-sized polyethylenimine(PEI)-modified polystyrene/Fe3O4/chitosan magnetic composite (PS/Fe3O4/CS-PEI) was developed as a novel adsorbent for the removal of Cu(II) ions from aqueous solutions. The PS/Fe3O4/CS-PEI microspheres with a diameter of similar to 300 nm can be highly monodisperse and conveniently separated from suspensions by a magnet due to their excellent magnetism. When the PS/Fe3O4/CS-PEI microspheres were used as an absorbent for the absorption of Cu(II) ions, the adsorption isotherms and adsorption kinetics well fitted the Langmuir model and the pseudo-second-order model, respectively. The maximum adsorption capacity was about 204.6 mg g(-1), which was higher than those of other chitosan adsorbents reported recently. The adsorption was considerably fast, reaching the equilibrium within 15 min. In addition, the adsorbed Cu(II) ions could be effectively desorbed using 0.1 mol L-1 NaOH solution, and the regeneration study proved that the composite microspheres could be repeatedly utilized without significant capacity loss after six cycles. All the results demonstrated that the synthesized sub-micron-sized magnetic PS/Fe3O4/CS-PEI composites can be used as an ideal adsorbent of Cu(II) ions for environmental cleanup applications. (C) 2016 Elsevier B.V. All rights reserved.