A systematic study of a series of MoxW1-xS2layered mixed crystals, with 0 ≥ x ≤ 1, grown by the chemical vapor transport method were carried out by using Raman scattering measurements. The peaks of the two dominant first-order Raman-active modes,A1gand E2g1 , and several second-order bands have been observed in the range of 150-500 cm-1. The peaks corresponding toA1gmode show one-mode type behavior while the peaks of E2g1 mode demonstrate two-mode type behavior for the entire series. The results can be explained on the basis of the atomic displacements for each mode. ForA1gmode only sulfur atoms vibrate and this give rise to a one-mode type behavior for the mixed crystals. For E2g1 mode metal atoms also vibrate as well as sulfur atoms, the mass difference of the vibrating Mo and W cations causes the two-mode type behavior of E2g1 mode. In addition, the observation of largest asymmetry and broadening ofA1gmode for Mo0.5W0.5S2has been attributed to random alloy scattering.