Optical vibrations confined in CdS nanocrystals (embedded in a glass film or forming a close-packed film with some organic-molecule links between them) have been studied experimentally, by means of FIR and Raman spectroscopies, and theoretically. The asymmetric Raman lineshape can be modelled considering resonant and non-resonant scattering on spherical modes with 1=0 (those with n>l are responsible for the low-frequency wing). A phonon-related dielectric response of the nanocrystal composites has been studied by measuring FIR reflectivity and transmission spectra. The theoretical consideration consists of the (i) calculation of the single-particle polarisability due to the confined 1=1 modes and (ii) including the dipole-dipole interaction between the particles. We show that, for the smallest particles, the FIR response has a bimodal structure, which disappears as the nanocrystal size increases. However, the experimentally observed bulk-CdS-like reflection band at 230–300 cm−1 is too broad and can not be explained by the model. Only making further assumptions, namely, of a fractal structure of the nanocrystal composites, enables us to fit well the experimental FIR spectra.