The applications of quaternary In0.15Sn0.85(Se0.95S0.05)2 (ITSS) crystals were investigated as a near-infrared (NIR) optoelectronic switching device, vacuum pressure sensor, and photocatalyst. The remarkable photoresponse is demonstrated by the NIR crystal-based ITSS photodetector for various applied external biasing voltage. The NIR photodetector exhibits fast switching with a photoresponsivity of 147 mA/W. The crystals were investigated as a vacuum pressure sensor in the vacuum range ranging from 0 mbar to −1033 mbar as a function of electrical resistance. The n-type grown quaternary crystals have a direct optical bandgap of 1.38 eV. The photocatalytic activity was assessed by varying the concentration of methylene blue (MB) and the characteristics of the photocatalytic process were computed using the Langmuir-Hinshelwood kinetic model. Raman spectroscopy was performed on the grown crystals at temperatures ranging from 98 K to 448 K, with a step of 50 K to study the structural stability. The Lorentzian function was fitted to the experimental data to determine the peak width and peak position. The quaternary ITSS crystals were grown by the mechanical alloying process. The stoichiometry and layered growth mechanism of grown ITSS crystals were confirmed through energy dispersive X-ray spectroscopy (EDS) with mapping and field emission scanning electron microscopy (FESEM), respectively. The hexagonal crystal structure was characterized by the powder X-ray diffraction (PXRD) pattern, and the electrical resistance was studied as a function of temperature.