In this research, we description synthesis of a novel silica-coated nano-Fe3O4 particles, which were successfully modified by diaminopyrimidine, and its physicochemical properties were characterized using FT-IR, XRD, TEM, FE-SEM, EDX, EDX-mapping, and TGA. The catalytic activity of this novel nano-catalyst was evaluated by three-component reactions for the preparation of pyranothiazolopyrimidines and 4H-pyrans under solvent-free conditions. Recyclability of the catalyst up to six consecutive rounds, atom economy, high yield and purity of desired products, and easy work-up method are some of the exciting features of this system that make it more favorable from a green chemistry point of view.