Layered double oxides (LDO) and gamma-Fe2O3 have been demonstrated to be promising adsorbents to remove radioactive elements from aqueous media. Herein, magnetic gamma-Fe2O3 nanoparticles decoration onto porous layered double oxides belts (gamma-Fe2O3/LDO) were fabricated by in situ solid-state thermolysis technique combined with Fe(III)-loaded layered double hydroxides as a precursor. The microstructure, chemical composition, and magnetic properties of gamma-Fe2O3/LDO were characterized in detail. The as obtained gamma-Fe2O3/LDO was employed as an adsorbent for the elimination of U(VI) from water. The adsorption process followed the Langmuir model with the maximal adsorption capacity of U(VI) onto gamma-Fe2O3/LDO being 526.32 mg.g(-1) at 303 K and pH 5, which surpassed pristine LDO and many other materials. The Fourier transformed infrared spectra and the X-ray photoelectron spectra analysis suggested that the interaction mechanism was mainly controlled by the surface complexation and electrostatic interactions. All in all, the gamma-Fe2O3/LDO with remarkable adsorption capacity, excellent regeneration, and easy magnetic separation opens a new expectation as a suitable material for the cleanup of U(VI) from contaminated water. (C) 2018 Elsevier Inc. All rights reserved.