<p>A new mixed ligands Cobalt complex of Schiff base and 2,2′-bipyridine was anchored onto the mesoporous MCM-41 to synthesize a highly efficient and reusable heterogeneous catalyst. The prepared heterogeneous catalyst was characterized by FT-IR, UV-DRS, PXRD, SEM-EDX, ICP-OES, HR-TEM, TGA, N₂ adsorption and desorption and ¹³C-CP-MAS-NMR. The Salen-Co-MCM-41-bipy complex has been found as a more promising catalyst for Knoevenagel condensation of aryl/alkyl malononitriles using different kind of aldehydes with malononitrile in EtOH/H₂O solvent mixture under room temperature with the yield upto 99%. The catalyst was performed well against a wide range of substrates, viz, the aldehydes of aryl, fused aryl, hetero and aliphatic compounds with a variety of substituents at various positions. Moreover, the effectiveness of our catalyst against large-scale reaction up to 2.5&#xa0;g of substrate was also explained. The catalyst is recovered by simple filtration and reused up to five times without any loss in activity. Hot filtration test was explored the heterogeneous nature of the recovered catalyst. Previous reports were compared and discussed to spotlight the efficiency of our catalyst.</p> Graphical abstract <p></p>