The direct fusion of 4-oxocyclohexanecarboxaldehyde dimethyl acetal (III) with cyanoguanidine provided the key intermediate, 2,4-diacetamido-5,6,7,8-tetrahydro-6-quinazolinecarboxaldehyde (XV), necessary for the synthesis of 5,8-dideaza-5,6,7,8-tetrahydroaminopterin (Ila). The conversion of XV to Ila was accomplished by the reductive alkylation of p-aminobenzoyl-L-glutamic acid with XV, followed by hydrolysis of the blocked intermediate XVIII to give the crystalline and chromatographically homogeneous Ila.