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In this article, we report on crystal growth, density functional theory (DFT) calculations, and scintillation properties of TlCaX $_{3} (X =$ Cl, Br, I). Crystals were grown by the vertical Bridgman technique in silica ampoules. Crystals of TlCaCl3, TlCaBr3, and TlCaI3 belong to the family of perovskites and have an orthorhombic crystal structure. All three compositions show bright emission under X-ray excitation peaking at 425, 470, and 545 nm, respectively. Light yield increases in the series Cl < Br < I [25 000–47 000 photons/MeV (ph/MeV)].