CdS films, both pure and doped with the alkali metals Na and K, with Cl and without it, obtained by the aerosol pyrolysis method from thiourea coordination compounds at a temperature of 250 to 500°C are investigated. The photoluminescence spectra and the dependence of the luminescence intensity on the duration of exposure of samples to a high-power UV radiation have been obtained. The doping of samples results in a tenfold increase in the intensity of the luminescence band in the visible spectrum range (650–850 nm) as compared to pure samples of CdS. Upon irradiation of samples by high-power UV radiation for 1 h, no noticeable change in the intensity of luminescence of CdS films was observed. This is indicative of the stability of the films under study against the action of UV radiation. The luminescent properties of the films, obtained pyrolytically using thiourea coordination complexes, are determined by the synthesis conditions as well as by the chemical nature of the original substances.