Pore size of mesoporous materials is crucial for their surface grafting. This article develops a novel multifunctional microsphere with a large pore size mesoporous silica shell (ca. 10.3 nm) and a magnetic core (Fe3O4), which is fabricated using cetyltrimethylammonium bromide (CTAB) as pore-forming agents, tetraethyl orthosilicate (TEOS) as silicon source through a sol-gel process. Compared with small pore size mesoporous silica magnetic microspheres (ca. 2-4 nm), the large pore size one can graft 447 mg/g amino groups in order to adsorb more heavy metal ions (Pb2+: 880.6 mg/g, Cu2+: 628.3 mg/g, Cd2+: 492.4 mg/g). The metal-loaded multifunctional microspheres could be easily removed from aqueous solution by magnetic separation and regenerated easily by acid treatment. The results suggest that the large pore size multifunctional microspheres are potentially useful materials for high effectively adsorbing and removing different heavy metal ions in aqueous solution. (C) 2013 Elsevier B.V. All rights reserved.