Structural dynamics of the layered CuCrS2 is investigated for the first time by using the Raman scattering method in 78–295 K temperature range on the samples synthesized by different methods. The Raman and IR spectra of CuCrS2 were simulated within the valence force field model with the LADY program. The results presented indicate that the lattice dynamics of CuCrS2 depends strongly on the real microstructure and technology of the sample preparation. The anomalous splitting of the A1 phonon mode might be due to presence of the α- and β-domains. Copyright © 2010 John Wiley & Sons, Ltd.