Sixteen 5-alkylamino-3,6-diaryl-2-thioxo-2,3,6,7-tetrahydrothiazolo[4,5-d]pyrimidin-7-ones 4a, 4b, 4c, 4d, 4e, 4f, 4g, 4h, 4i, 4j, 4k, 4l, 4m, 4n, 4o, 4p were designed and easily synthesized via a tandem aza-Wittig reaction. The iminophosphorane 2, obtained from reaction of 1 with triphenylphosphine, hexachloroethane and Et3N, reacted with aromatic isocyanate to give carbodiimide 3. carbodiimide 3 reacted with alkylamines to provide the title compounds in 45–61% isolated yields in presence of catalytic amount of ethoxide. The structures of compounds 4 were confirmed by...