Polarized Raman spectra obtained from carefully characterized single crystals of ZnIn,S,, Zn,In,S,, and Zn,In,S, are reported. The low-frequency Raman spectra clearly differentiate between the compounds, whereas at high frequencies the vibrational features are less sensitive to the actual crystal structure. The results are interpreted on the basis of a molecular-like picture based on the intrinsic cationic disorder.