In this work, the combined experimental and theoretical study on molecular and vibrational structure of 4-chlorotoluene (4CT) was studied based on Hartree-Fock (HF) and density functional theory (DFT) using the hybrid functional B3LYP. The Fourier Transform Infrared (FTIR) and Fourier Transform Raman (FT-Raman) spectra of 4CT were recorded in the solid phase. The optimized geometry was calculated by HF and B3LYP methods with 6-31G(d,p) and 6-311++G(d,p) basis sets. The harmonic vibrational frequencies, infrared intensities and Raman scattering activities of the title compound were performed at same level of theories. The thermodynamic functions of the title compound was also performed at HF/6-31G(d,p) and B3LYP/6-311++G(d,p) level of theories. A detailed interpretation of the infrared and Raman spectra of 4CT was reported. The observed and the calculated frequencies are found to be in good agreement. The experimental spectra also coincide satisfactorily with those of theoretically constructed spectrograms.