1.1-bis(4-chlorophenyl)-2,2,2-trichloroethane (DDT) is of concern in water treatment because of its persistence and health effects. A new concept is proposed to synthesize hexagonal mesoporous silica (HMS) with magnetic functionalization for DDT removal from aqueous media. Fe3O4 nanocrystals were synthesized by a low-temperature solvothermal process, and then encapsulated in mesoporous silica through a packing approach, forming core-shell structured Fe3O4@HMS microspheres. The synthesized materials were characterized by X-ray diffraction (XRD), transmission electron microscopy (TEM) and nitrogen adsorption-desorption techniques. The results indicate that the silica shell conserves mesoporous structure after the removal of surfactant templates. Different from previous studies, the thickness, pore volume and surface area of silica shell can be controlled by adjusting the reaction condition. These Fe3O4@HMS materials show high adsorption capacity and fast adsorption rate for DDT. Because of the useful magnetic property and unique mesoporous structure, the synthesized materials provide a fast, convenient and highly efficient means to remove DDT from aqueous media. Crown Copyright (C) 2009 Published by Elsevier B.V. All rights reserved.