Eu:CaAl2O4, Eu:SrAl2O4, and Eu:BaAl2O4 crystals with various dopant concentration were synthesized by the optical floating zone method, and the photoluminescence, scintillation, and afterglow properties were investigated. Under X-ray irradiation, Eu:CaAl2O4 Eu:SrAl2O4, and Eu:BaAl2O4 exhibit a broad emission band at 440, 520, and 500 nm due to 5d-4f transitions of Eu2+, respectively. The decay time constants are consistent with the typical values of 5d-4f transitions of Eu2+. Photoluminescence quantum yield and scintillation light yield were evaluated, and each property was compared to comprehensively understand the characteristics.