Adsorption of cationic methyl green (MG) on nontreated (AB) and purified (AP) natural Sejnane clay type was studied in an equilibrium batch process. This work reported the application of kaolinite-rich heterogeneous clay for the removal of a cationic dye. Effects of contact time, initial dye concentration, mass adsorbent, pH, and temperature on the MG removal were checked. The adsorbent before and after adsorption processes was characterized by X-ray diffraction (XRD), scanning electron microscopy (SEM), Fourier transform infrared (FTIR), and atomic adsorption spectrophotometer. Equilibrium data were mathematically modeled using the Freundlich, Langmuir, and intraparticle diffusion models. Kinetic of adsorption was determined by pseudo-first-order and pseudo-second-order models. The free energy (ΔG°), standard enthalpy (ΔH°), and standard entropy (ΔS°) were calculated. A fast increase in the equilibrium removal of the cationic dye was obtained at a pH ranging between 3 and 11 and moderate temperature. This rapid MG adsorption proved the efficiency of kaolinite clay in cationic dye removal. Decolorizing yields were 73.3% for AB and 99.8% for AP. Thus, the adsorption capacity of purified clay was clearly higher than of H₂SO₄ and thermic activated clays. The data more closely resembled a pseudo-second-order model process, and the clay had reasonable Freundlich adsorption capacity. Adsorption process was endothermic and spontaneous chemisorption. SEM analysis showed that the adsorbed MG had remarkably changed the morphology of raw and purified clay surface. The low desorption rates confirmed effectiveness of this type of material for the retention of methyl green molecules. Thus, tested clays have no environmental impact.