Single crystals of Bis(thiourea) cadmium chloride (BTCC), and Tris(thiourea) zinc sulphate (TZnS) have been grown from saturated aqueous solution by slow evaporation method at room temperature. The laser Raman and FT‐IR spectra on these crystals are recorded in the frequency range 50–4000 cm⁻¹. The spectral data of BTCC and TZnS are interpreted on the basis of thiourea crystal vibrational data. The vibrational frequencies in the FT‐IR and Raman spectra of BTCC and TZnS establish that ZnSO₄ and CdCl₂ metal complex are coordinated with thiourea by the metal to sulfur bonds. The effect of the metal complexation on thiourea molecule and nature of bands due to different vibrational modes have been discussed. The lattice vibrational frequencies changes have also been observed and analyzed.