A combined sol-gel-cum-hydrothermalmethod has been employed to synthesize novelmonometallic (Mn, Fe, Co) and bimetallic (Co-Fe, Mn-Co, Fe-Mn) nanoparticles loaded onto Al₂O₃−MCM-41. Powder XRD, N2 sorption, field emission scanning electron microscopy (FESEM) and high resolution transmission electron microscopy (HRTEM) measurements show that the materials possess mesoporosity, high surface area and nanosize. Monometallic Fe, Co and Mn @Al₂O₃−MCM-41 and bimetallic Co-Fe, Fe-Mn and Mn-Co @Al₂O₃−MCM-41 materials were tested for methylene blue remediation from aqueous media. In the present study, Co-Fe@Al₂O₃−MCM-41 was found to be an excellent adsorbent. The adsorption efficiency of Co- Fe@Al₂O₃−MCM-41 has been studied as a function of adsorbent dose and pH of the solution. Maximum adsorption of methylene blue was obtained at high pH values of the solution. Framework mesoporosity, high surface area, and narrow pore distribution are the key factors for an efficient adsorption of methylene blue onCo-Fe@Al₂O₃−MCM-41.