In this work, a combined theoretical and experimental study of binary mixture of liquid p-methylbenzaldehyde (PMBz) is reported using ab initio calculations as well as Raman and IR spectroscopies. The purpose of this study was twofold: firstly, to describe the interaction of PMBz in terms of bonding energies and preferred geometries; and secondly, to characterize the spectroscopic effects on the vibrational modes of PMBz in the binary mixture of different polar and nonpolar solvents. The three vibrational modes, namely, carbonyl stretching, ν(C-CH 3 ) and aldehydic (C-H) vibrations have been analyzed in all the three solvents in different concentrations. The dependence of Raman linewidth on the concentration of PMBz of these modes was also taken into account. By analyzing the peak position and linewidth of these modes, it is seen that the solute-solvent interaction is stronger in BuOH and 1,2 dichloroethane (DCE) because of the hydrogen-bonding interaction between these molecules. The formation of C-H· · ·O hydrogen bonds in liquid p-methylbenzaldehyde is also investigated by Gaussian fitting. The ab initio calculations suggest several possible dimer configurations.