The paper studies the amplitude and spectral-kinetic behavior of pulsed X-ray and cathodoluminescence of non-alloyed zinc selenide (ZnSe) single crystals and those alloyed by gallium, tellurium and samarium. At 300 K, the spectra of pulsed cathodoluminescence of pure ZnSe single crystals show a 490 nm illumination at ~20 ns pulse time. Two spectral bands are observed in alloyed ZnSe single crystals, band edge at ~477 nm and with maximum at ~600 nm at a pulse time of ~20 ns and ~5 μs, respectively. The intensity ratio of these peaks depends on the electron-beam energy density and the geometry of spectrum measurements. X-ray luminescence spectra of the alloyed ZnSe single crystals show an ~600 nm illumination, the intensity of which depends on the type of impurity. The possibility of applying the pure and alloyed ZnSe single crystals is discussed herein for the development of amplitude-time characteristic sensors of electron beams and X-ray radiation energy ranging from tens to hundreds of kiloelectronvolts.