Abstract: A systematic optical characterization of a series of Mo1-xWxS2 (0 ≤ x ≤ 1) layered mixed crystals grown by chemical vapour transport method were carried out by using piezoreflectance (PzR) and Raman scattering measurements. From a detailed lineshape fit of the PzR spectra over an energy range from 1.6 to 5.0 eV, the energies of the band-edge excitonic and higher lying interband transitions were determined accurately. The transition energies and their splittings vary smoothly with the tungsten composition x indicating that the nature of the band structure is similar for the Mo1-xWxS2 series compounds. The peaks of the two dominant first-order Raman-active modes, and , and several second-order bands are observed in the range of 250-450 cm-1. The peaks corresponding to mode show a one-mode type behavior, while the peaks of mode demonstrate two-mode type behavior for the entire series of Mo1-xWxS2 crystals. These behaviors were discussed on the basis of the lattice vibrational properties of 2H-MoS2 and 2H-WS2 compounds.