Magnetic ferrite (Mg-doped bismuth ferrite) and its clay-based composite (Mg-doped bismuth ferrite-bentonite) were prepared by self-combustion method utilizing glycine as fuel and served for the removal of methyl orange (MO) from aqueous solutions. The ferrite-based adsorbents were characterized by the measurement of specific surface area (BET), scanning electron microscopy (SEM), Fourier Transform Infrared Spectroscopy (FTIR), X-ray diffraction (XRD). The different experimental parameters that affect the performance of this reaction such as: temperature, contact time, initial dye concentration and mass of adsorbent were investigated. The point of zero charge pH (pHPZC) was determined for the two adsorbents. Langmuir and Freundlich adsorption models were employed to provide a description of the equilibrium isotherms. Adsorption tests showed that the equilibrium time is a function of the initial concentration of dye. The adsorption kinetic study indicated that the equilibrium adsorption is established after 300 minutes for Mg-doped bismuth ferrite, while it is established after 180 minutes for Mg-doped bismuth ferrite-bentonite composite. Furthermore, this suggests that the adsorption of MO on both adsorbents can be perfectly described by pseudo-second order kinetics. The maximum adsorption capacity determined by the mathematical model of Langmuir is equal to 181.8 mg.g-1 for Mg-doped bismuth ferrite and to 188.7 mg.g-1 for its composite, at 298 K. Adsorption isotherms shows that the Freundlich model perfectly represents adsorption of methyl orange to the prepared Mg-doped bismuth ferrite. The ferrite/bentonite composite has 2-50 nm-sized pores and is indeed a mesoporous material. The small pores observed on the surface of the adsorbents are in line with type IV isotherm, with possible capillary condensation of the adsorbate. Moreover, Langmuir model seems to be the most suitable model for the absorption of methyl orange on the Mg-doped bismuth ferrite-bentonite composite. The thermodynamic parameters related to the sorbent/adsorbate system indicate that adsorption is spontaneous and exothermic. The determination of isosteric heat of adsorption suggested that it is indeed a physisorption characterized by weak intermolecular forces between MO and the surface.