Abstract:The infrared spectroscopic investigations for the =CH and NH vibrations and the effect of substitution at different positions in the phenyl rings of 2-amino-4,6-diphenyl-3,6-dihydropyrimidines have been described. The CH stretchings were observed between 3070-3060 cmG 1 . The observed frequencies differ for -NH bending and the =CH and -CH stretching vibrations, and the difference between the two frequencies is larger than the predicted differences between scaled frequencies. It has been observed that the substitution of phenyl rings with -OH, -OCH 3 , -NO 2 and -Cl groups, further complicated the elucidation of the spectra. The electronic transitions in the UV spectra were observed to be hypsochromic (blue shift) when a powerful electron donor group is present in the heterocyclic nucleus. Other electronic transitions were observed in the ultraviolet spectra to check the presence of B-B * and n-* transitions in these compounds.