Blocked isocytosine isocyanates are conveniently obtained by the reaction of 1,1′‐carbonyldiimidazole (CDI) with isocytosines. The resulting precursors for quadruple hydrogen‐bonded structures can be isolated and stored for further use. Reaction with either aliphatic or aromatic amines gives the corresponding mono‐, bi‐, or trifunctional ureidopyrimidinone derivatives in good to excellent isolated yields. (© Wiley‐VCH Verlag GmbH & Co. KGaA, 69451 Weinheim, Germany, 2004)