Harmaline belonging to a family of harmala is a fluorescent psychoactive indole alkaloid. The FTIR and FT-Raman spectra of Harmaline have been recorded in region 4000__ampersandsignndash;400 cm-1 and 4,000__ampersandsignndash;100 cm-1 respectively. The experimental frequencies recorded are compared with vibration frequencies calculated using Gaussian software by employing HF and DFT functional at B3LYP/6-31G(d,p) basis set. The electronic properties of the molecule have been studied by recording UV__ampersandsignndash;Visible spectrum of the compound. Also, highest occupied (HOMO) and lowest unoccupied molecular orbital (LUMO) energies have been calculated at DFT/B3LYP/6-31 G (d,p) level. These calculations showed that there exists energy transfer in the molecule. Mulliken population analysis and thermodynamic properties of title compound have been analyzed and tabulated.