In this work, the vibrational spectral analysis was carried out by using FT-IR and FT-Raman spectroscopy in the range 400-4000 cm-1 and 100-1900 cm-1 respectively, for Thiosemicarbazone of m-nitrobenzaldehyde molecule. The potential energy curve shows that molecule molecule has one stable structure. The molecular structure, fundamental vibrational frequencies and loudness of the vibrations bands were interpreted with the aid of structure optimizations and normal coordinate force field calculations-based density functional theory (DFT) and ab initio HF methods and different basis set combination. The outcomes of the computation were put on to simulated spectra of the title compound, which show excellent agreement with observed spectra. The scaled B3LYP/6-311++G (d -p) results show the best agreement with the experimental values over the other method. The energy and oscillator strength calculated by Time-Dependent Density Functional Theory (TD-DFT) complements with the experimental findings. In addition, molecular electrostatic potential and thermodynamic properties of the title compound were performed. Mulligan and natural charges of the title molecule were also calculated and interpreted.