Recently, magnetic sorbents have received considerable attention because of their excellent segregative features and sorption capacities. Herein, attapulgite/iron oxide magnetic (ATP/IOM) composites were prepared and characterized. The sorption results indicated that ATP/IOM composites were superior to ATP and iron oxides individually for the removal of U(VI) from aqueous solution. Based on X-ray photoelectron spectroscopy (XPS) analysis and surface complexation model, the main sorption species of U(VI) on ATP were =X(2)UO(2)(0) below pH 4.0 and =S(s)OUO(2)(+),=S(w)OUO(2)CO(3)(-), and =S(w)OUO(2)(CO(3))(2)(3-) above pH 5.0. However the prevalent species on ATP/IOM composites were =SsOUO(2)(+) and =SwOUO(2)(CO(3))(2)(3-) over the observed pH range. ATP/IOM composites are a promising candidate for pre-concentration and immobilization of radionuclides from large volumes of aqueous solutions, as required for remediation purposes. (C) 2011 Elsevier B.V. All rights reserved.