In this investigation, Maghnia (Ma) and Mostaganem (Ms) bentonite clays, mined from west Algeria, with no prior affinity for anionic dyes, were modified by simple ion exchange with aqueous Fe3+ solutions, followed by calcination at 500°C. The resulting materials, Fe-Ma and Fe-Ms, respectively, were employed as adsorbents for methyl orange. The starting materials and the two adsorbents were characterized by X-ray diffraction, N2 adsorption–desorption isotherms, Brunauer–Emmett–Teller specific surface area and X-ray fluorescence and by determining the point of zero charge. The effects of various variables, such as initial dye concentration, contact time, adsorbent dose, initial pH and adsorption temperature, were studied. The kinetics were well described by the pseudo-second-order model and the mechanism was determined from the intraparticle diffusion model, while corresponding isotherms fitted better to the Freundlich model. Thermodynamic parameters showed that the adsorption process was endothermic, spontaneous and physical in nature, accompanied by an increase of entropy.