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Inorganic scintillation crystals have been widely used in applications of high-energy physics, nuclear medical imaging, industrial nondestructive inspection, etc. In this work, a single crystal Ba₃Y(PO₄)₃ (BYP) with 1.0 at% Ce³⁺-doping concentration was first grown by the Czochralski method, and the electronic structure was calculated using first principles based on density functional theory. In addition, a series of Ce³⁺-doped BYP phosphors were synthesized, and the fluorescence emission under UV excitation was measured through low-temperature spectroscopy, containing double-peaked emission from 5d–4f transition and self-trapped exciton recombination. A comparison of the UV and X-ray-excited fluorescence spectra reveals the existence of oxygen vacancies as well as F+ centers in the crystal. The air annealing of the crystal effectively reduces the thermoluminescence defects but reduces the emission intensity under UV or X-ray excitation. The BYP:Ce crystal shows a fast decay lifetime of 15.5 ns, and the fast component is as short as 8 ns. The results show that the Ce³⁺-doped BYP crystal has potential as a kind of scintillator with fast decay properties.