The pyrimidines fused with pyrrole ring, pyrrolopyrimidines, showed broad applicability in medicinal chemistry. Herein, we synthesized the new derivatives (8 examples) of pyrrolo[1,2-a] pyrimidine containing 1,3-indandione skeleton by the use of triethylammonium thiolates, methyl iodide, and ketene aminals via a one-pot three-component reaction. Scheme 1. Synthesis of pyrrolo[1,2-a]pyrimidine containing 1,3-indandione skeleton.