This article presents the results of an experimental investigation of the energy spectra of charge carrier traps in undoped high-resistivity ZnSe single crystals. Fourteen peaks were found in the thermostimulated luminescence spectra of the ZnSe samples at temperatures between 8 K and 450 K, and the thermal activation energies of the charge carrier traps were estimated for the most intense peaks. It was found that the energy spectra of the charge carrier traps in ZnSe exhibit oscillatory regularity, and the energy of a vibrational quantum was estimated to be ω = 206 cm −1 , which is in good agreement with the vibrational mode in the Raman spectrum. Additionally, a linear relationship was observed between the thermal activation energies of the charge carrier traps and the temperature positions of the maxima in the thermostimulated luminescence of ZnSe.