Recognition of DNA duplexes by triplex forming oligonucleotides (TFO) is limited to DNA homopurine sequences. As a first step to overcome this limitation we report here NMR recognition studies of the C· G base pair by new heterocyclic systems, derived from benzimidazole and benzoxazole units bearing an urea donor moiety, designed to bound to the 4-amino group of the cytosine and the O4-and N7-atoms of the guanosine bases, ...