The (E)-N'-((Pyridin-2-yl)methylene)benzohydrazide (PMBH) was synthesized and its structural characterization was made by the X-ray diffraction method. The spectral investigations such as FT-IR, FF-Raman and UV-Visible spectra were carried out. The recorded X-ray diffraction bond parameters were compared with theoretical values calculated at B3LYP/6-311++G (d, p) level of theory. The observed spectral results were compared with the computed wavenumber. The vibrational assignments were carried out by the total energy distribution (TED) method. The first order hyperpolarizability, intra-molecular charge transfer and band gap energy were studied using B3LYP/6-311++G (d, p) calculation. The electronic transition was studied using UV-Visible spectrum and the observed values were compared with the theoretical values. The electrostatic potential surface of the title molecule was also analyzed using the same level of basis set. (C) 2014 Elsevier B.V. All rights reserved.