This paper describes the synthesis, self-assembly, and characterization of a new class of highly stable hydrazide-based quadruply hydrogen-bonded heterodimers. All of the hydrazide-derived heterodimers possess the complementary ADDA-DAAD hydrogen- bonding sequences. Hydrazide derivatives 1, which has two intramolecular S (6) RO⊙⊙⊙ HN hydrogen bonds, and 2 complex to afford two fastly exchanging isomeric heterodimers ...