High optical quality nonlinear crystals of solid solution GaSe1−xSx, x=0, 0.05, 0.11, 0.22, 0.29, 0.44, 1 were grown by modified Bridgman method with heat field rotation. Ordinary and extraordinary wave dispersion was studied in detail as a function of sulfur content by terahertz time-domain spectroscopy (THz TDS) in the 0.3–4 THz range