The structural, electronic, mechanical properties, and frequency-dependent refractive indexes of GaSe 1−x S x (x = 0, 0.25, and 1) are studied by using the first-principles pseudopotential method within density functional theory. The calculated results demonstrate the relationships between intralayer structure and elastic modulus in GaSe 1−x S x (x = 0, 0.25, and 1). Doping of ε-GaSe with S strengthens the Ga-X bonds and increases its elastic moduli of C 11 and C 66 . Born effective charge analysis provides an explanation for the modification of cleavage properties about the doping of ε-GaSe with S. The calculated results of band gaps suggest that the distance between intralayer atom and substitution of S Se , rather than interlayer force, is a key factor influencing the electronic exciton energy of the layer semiconductor. The calculated refractive indexes indicate that the doping of ε-GaSe with S reduces its refractive index and increases its birefringence.