Abstract The synthesis of 4, 5, 7, 8-tetrahydro-6H-imidazo [4, 5-e][1, 4] diazepine-5, 8-dione and its several 1-and 3-alkyl (aralkyl) derivatives 2 has been reported. Mechanistic explorations of the final synthetic step as well as structural confirmation of a final product 2d by single-crystal X-ray diffraction analyses have also been presented.