An illite-montmorillonite clay from Naima, IMN (Algeria) was treated via physical and chemical treatment (TIMN) and investigated for the removal of methylene blue. IMN and TIMN clays were characterized by XRD, XRF, SEM-EDS, DSC-GA, FTIR and DC electrical conductivity methods. To analyze the sorption behavior of MB on the clays, a mechanistic model for interpreting the sorption data was developed. IMN clay revealed high sorption capacity (1.925 × 10−2 kg kg−1) for MB in 60 min. The pseudo-second-order model had a very good agreement to describe the MB adsorption process. The adsorption capacities, qe,exp, of 4.327 × 10−2 and 4.914 × 10−2 kg kg−1 for IMN and TIMN, respectively, were obtained. The free energy from the D–R model from adsorbing MB using IMN and TIMN ranged from 1.581 to 0.745 × 10−3J mol−1, respectively, suggesting that the process is physisorption. Besides, the sorption process was more sensible to temperatures that increase was beyond 40 °C causing a decrease in adsorption capacity, indicating that the adsorption reaction of MB onto IMN was exothermic. The adsorption mechanism of I/M clay to remove MB was likely based on hydrogen bonding, electrostatic attraction, cation exchange and n–π interaction. These results proved that TIMN was a promising adsorbent for removing MB from its simulated wastewater.