The photocatalytic potential of chlorophyll has been investigated for the facile synthesis of dihydropyrimidinones utilizing concentrated solar irradiation towards sustainable energy solutions. This, one-pot, multicomponent Biginelli reaction, which involves a photoinduced electron transfer (PET) mechanism, affords a green and efficient approach for the transformation of the commercial aldehydes, β-keto ester and urea into valuable 3,4-dihydropyrimidin-2(1H)-ones with wide substrate scope and diversity. These improved reaction conditions allow the formation of a variety of substituted dihydropyrimidinones with high yields and purity in a short duration of time and mild reaction conditions.