Transition metal dichalcogenides (TMDCs) have attracted global interest in recent years due to their optoelectronic characteristics and tunable bandgap energies. Due to their potential use in photovoltaic devices, photodetectors, and field effect transistor (FET) recording systems, single crystalline semiconductors of TMDC family have attracted a lot of attention. In the present article, the direct vapour transport technique was used to synthesis the InxMo1-xS2 (x = 0, 0.05, and 0.1) crystals. The purity and distribution of all the elements were investigated by EDAX mapping. The power X-ray diffraction technique examine the grown crystals have hexagonal lattice structure. The structure of all the crystals was investigated by scanning electron microscopy (SEM). The in-plane E2g and outer-plane A1g vibration modes were studied through Raman spectra. Photodetectors based on InxMo1-xS2(x = 0, 0.05, and 0.1) crystals show the self-powered photoresponse under white light source at 100 mW/cm2power intensity.