The dielectric and impedance spectra of TlGaSe2 crystals have been studied at temperatures in the 100–500 K range in the alternating current (AC [Formula: see text]1 V). It has been shown that the conductivity of TlGaSe2 crystals is mainly an ionic characteristic at temperatures above 400 K. The well-defined peak at the frequency dependence of the imaginary part of impedance [Formula: see text] is observed in the 215–500 K temperature range. In a constant field, there occurs a significant decrease in electrical conductivity [Formula: see text] in due course. The ionic contribution to conductivity (76% at [Formula: see text]) has been estimated from a kinetic change in electrical conductivity [Formula: see text] under the influence of a constant electric field. The diagram analysis in a complex plane [Formula: see text] has been conducted by applying the method of an equivalent circuit of the substation. It has been determined that the average relaxation time of the electric module of the sample is [Formula: see text].