A single-step process for the preparation of 2-amino-7-chlorothiazolo [5, 4-d] pyrimidines, 2, was achieved by the reaction of the commercially available 4, 6-dichloro-5-aminopyrimidine 1 with isothiocyanates. This mild reaction accommodates a variety of functionalized isothiocyanates and proceeds in good to excellent yields. The utility of such intermediates is exemplified by subsequent reaction with alkyl or arylamine nucleophiles to afford novel, ...