Developing efficient and environmentally sustainable pathways is a fascinating focus within the field of green chemistry. In this study, a bimetallic Co-Mg metal–organic framework (Co-Mg MOF) was synthesized through solvothermal conditions using Co2+ and Mg2+ ions along with NH2BDC (2-amino terephthalic acid) as a rigid ligand. Comprehensive characterization was performed using powder X-ray diffraction (PXRD), nitrogen adsorption–desorption isotherm (BET method), thermogravimetric analysis (TGA), elemental mapping, and inductively coupled plasma (ICP) techniques. The as-synthesized catalyst exhibited great catalytic performance in the Knoevenagel condensation of malononitrile and benzaldehyde, possibly due to its abundance of basic and acidic sites. Besides this, the bimetallic MOF catalyst demonstrated superior catalytic activity compared to its single-metal counterparts (Co-MOF and Mg MOF), this enhanced performance is likely due to the synergic effect of incorporating Mg2+ into the Co-MOF framework. With the optimization of reaction conditions, a significant yield of the final products (involving various aldehydes and malononitrile) was achieved at room temperature within a short duration. The as-synthesized catalyst represented good stability and recyclability through the reaction process even after the 4th run. The results showed that the as-synthesized bimetal Co-Mg MOF exhibited superior potential as a catalyst in the Knoevenagel condensation reaction, in the presence of green solvent (ethanol).