An effective procedure for the synthesis of amino-functionalized fullerene with diethylenetriamine (C60-NH2) is described. The obtained material was characterized by Fourier-transform infrared spectroscopy (FT-IR), X-ray diffraction (XRD), scanning electron microscopy (SEM), energy dispersive X-ray spectroscopy (EDS), elemental analysis (CHN), thermogravimetric analysis (TGA) and X-ray photoelectron spectroscopy (XPS). The catalytic activity of C60-NH2 was studied in multicomponent reactions (MCRs) for the synthesis of chromene and pyrimidine derivatives. The results revealed that C60-NH2 was very effective and the desired chromene and pyrimidine products were isolated in good to excellent yields 78–97% and 81-98%, respectively. Moreover, the C60-NH2 catalyst could be recycled and reused for at least 8 runs without substantial loss in its activity, which makes our procedure environmentally benign. Antibacterial behavior of some of the synthesized products was studied for Gram-positive and Gram-negative bacteria using disk and well diffusion methods. The chromene 4g showed a good antibacterial activity against both bacterial strains Staphylococcus aureus (S. aureus) and Serratia marcescens (S. marcescens). A good antibacterial activity was also detected for chromene 4o and pyrimidine 7j against S. aureus. The chromene 4m, 4n and pyrimidine 7i compounds displayed a good activity against Micrococcus luteus (M. luteus) as a Gram-positive bacterium.