A set of esters of the bis-Biginelli type were produced under the Green Chemistry Protocol, employing solventless conditions, using infrared irradiation as activating source and moreover in the absence of catalyst. The products were studied by mass spectrometry (electron impact, linked scans and high resolution) in order to characterize them and complementary to establish a validated fragmentation pattern. In addition, the vasodilatorily effect of the title molecules, in comparison with nifedipine, was also evaluated. Furthermore, the corresponding thermal analyses and X-ray diffraction patterns, for the obtained products, were carried out in order to explain the crystalline or amorphous forms, as well as their ambiguous melting points.