Thieno[2,3-d]thiazoles were prepared by reaction of 4-chlorothiazole-5-carbaldehydes or 4-chlorothiazole-5-carbonitriles with either ethyl 2-mercaptoacetate or 2-mercaptoacetamide. The 6-aminothieno[2,3-d]thiazole-5-carboxamides obtained were converted into the corresponding thiazolo[4',5';4,5]thieno[3,2-d]pyrimidin-5(6H)-one by treatment with triethyl orthoformate in acetic anhydride. With phosphoryl chloride these gave the 5-chloro-derivative, which underwent displacement of the chlorine-atom when allowed to react with various amines. Reductive dechlorination of 5-chlorothiazolo[4',5';4,5]thieno[3,2-d]-pyrimidine gave the parent heterocycle.