Abstract The isothiocyanate 3, obtained from aza??Wittig reaction of iminophosphorane 2 with CS2, reacts with phenylhydrazine to give thiosemicarbazide 4. Reactions of 4 with alkyl halides in the presence of K2CO3 directly provided 2??alkylthio??4H??imidazol??4??ones 6 in good yields.