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It is shown that the replacement of a part of sulfur atoms with selenium atoms in a TlInS2 single crystal stimulates the formation of a single-phase state with a monoclinic structure (space group [Formula: see text]/[Formula: see text] in TlInS[Formula: see text]Se[Formula: see text] ([Formula: see text]). Irradiation with 2 MeV electrons and a fluence of [Formula: see text] electron/cm2 of powder TlInS[Formula: see text]Se[Formula: see text] ([Formula: see text]) leads to an increase in the crystallite size from 56.5 nm to 65 nm, which is most likely associated with a decrease in the interface. The difference between the surface morphology of the synthesized TlInS[Formula: see text]Se[Formula: see text] ([Formula: see text]) single crystal and the surface morphology of the TlInS2 single crystal is established, which consists in a decrease in the height and width of the roughness in TlInS[Formula: see text]Se[Formula: see text] ([Formula: see text]). Irradiation of a TlInS[Formula: see text]Se[Formula: see text] ([Formula: see text]) single crystal with electrons with a fluence of [Formula: see text] electron/cm2 does not lead to a change in the height of the tubercle on its surface, and the average value of its width increases more than ten-fold. The identity of the peaks in the Raman spectra of the TlInS[Formula: see text]Se[Formula: see text] ([Formula: see text]) single crystal before and after its irradiation with electrons with an energy of 2 MeV and upto a fluence of [Formula: see text] electron/cm2, along with the absence of a shift of the peaks, indicates the radiation resistance of the TlInS[Formula: see text]Se[Formula: see text] ([Formula: see text]) single crystal.