The molecular geometry, vibrational frequencies, gauge-including atomic orbital (CIAO) H-1 and C-13 chemical shift values of 4-cyanobenzaldehyde isonicotinoyl-hydrazone monohydrate in the ground state have been calculated by using the Hartree-Fock (HF) and density functional method (DFT/B3LYP) with 6-31++G(d,p) basis set. Furthermore, this structure has been confirmed by IR, C-13 and H-1 spectroscopy. The results of the optimized molecular structure are presented and compared with the experimental X-ray diffraction. The computed vibration frequencies are used to determine the types of molecular motions associated with each of the experimental bands observed. C-13 and H-1 NMR data were calculated by means of the methods of GIAO, CSGT, and IGAIM. Calculated chemical shift values are compared with the experimental 4-cyanobenzaldehyde isonicotinoyl-hydrazone monohydrate. (C) 2010 Elsevier B.V. All rights reserved.