In this work, we studied the effect of electron irradiation on the structure and morphology of the surface of a single crystal and polycrystal TlIn1-xCrxS2 (x=0.01). Irradiation of a TlIn1-xCrxS2 single crystal with electrons with an energy of 2 MeV and a fluence of 2×1017 electron/cm2 leads to an increase in the maximum value of the mean arithmetic deviation of the profile from Ra=5.4 nm to Ra=25.2 nm, and also leads to an increase in the height of the average roughness from Rz=72.0 nm to Rz=152.9 nm. Irradiation of powder TlIn1-xCrxS2 with electrons with a fluence of 2×1017 electron/cm2 promotes an increase in the crystallite size from 36.87 nm to 41.76 nm, which is most likely associated with a decrease in size of the interface.