A new series of liquid-crystalline tapered hydrazide derivatives with an amino head group, e.g. N-(3,4,5-trialkoxylbenzoyl)-N'-(4'-aminobenzoyl) hydrazine (Dn, where n is the number of carbon atoms in the alkyl chains, n=6, 8, 16), were designed and synthesized. Results of H-1 NMR diluting experiment and FTIR spectroscopy revealed that the amide protons of the central hydrazide group in On participated in intermolecular double hydrogen bonds based on C=O and -NH in liquid crystalline phase. Investigations on the liquid crystalline properties showed that the D6 exhibited non-mesophase, D8 exhibited monotropic hexagonal columnar mesophase, while D16 exhibited enantiotropic oblique columnar mesophase with increasing the length of the terminal chains. (C) 2012 Elsevier B.V. All rights reserved.