In this paper, we have prepared Dy-doped MgAl2O4 single crystals by the Floating Zone (FZ) method and investigated photoluminescence (PL), scintillation, and thermally stimulated luminescence (TSL) properties. In PL and scintillation, origins of luminescence at around 480, 580, and 660 nm of synthesized crystals were assigned to the 4f-4f transitions of Dy3+. In TSL, three glow peaks at around 50, 220, and 350 degrees C were observed, and these peaks were attributed to cation antisites and V center. The 0.1 % Dy-doped MgAl2O4 single crystal showed the highest intensity in TSL glow curves among the prepared crystals and higher sensitivity than those in ceramic-form MgAl2O4.