AbstractFe3O4 nanoparticles were synthesized and functionalized by molybdenum aurintricarboxylic acid. Complex physicochemical characteristics of the catalyst were investigated by various methods such as infrared spectroscopy, X‐ray diffraction, scanning electron microscopy, vibrating sample magnetometry, and X‐ray energy diffraction spectroscopy. The results confirmed the spherical morphology, nanoscale size, magnetic properties, and the presence of the desired elements in the synthesized catalyst. Efficiency of the catalyst was determined by the synthesis of dihydropyrimidinone derivatives via Biginelli condensation. Under optimal conditions, a variety of dihydropyrimidinones derivatives were synthesized with good and excellent yields. The magnetic nature of the catalyst, easy separation of the reaction mixture, and catalyst reusability are the advantages of this work. The use of solvent‐free conditions is the other advantage.