New fluorescent compounds, 2-substituted indeno[1,2-d]pyrimidin-5-ones () were synthesized in good yield by the reaction of 2-[bis(methylsulfanyl)methylene]indan-1,3-dione () with the respective amidine derivatives [guanidine carbonate (), acetamidine hydrochloride (), S-methylisothiourea sulfate (), and S-benzylisothiourea sulfate ()]. 4-Substituted amino-2-aminoindeno[1,2-d]pyrimidin-5-ones () were synthesized by a one-pot reaction of , and the respective amine compounds () in pyridine. These fused pyrimidine derivatives showed fluorescence in the solid state.