The undoped and Ce-doped MgAl2O4 single crystals were synthesized by the floating zone method equipped with four xenon arc lamps, and the photoluminescence (PL), scintillation, and dosimetric properties were investigated. The Ce-doped crystals showed PL emission peaks at around 420 and 720 nm. The former was ascribed to the 5 d-4f transition of Ce3+ ion, and the latter was ascribed Mg deficiency. The PL decay time profiles of the Ce-doped crystals exhibited the fast decay, and the decay time constants were the typical value of others Ce-doped materials. Thus, the decay time constants were attributed to the 5 d-4f transitions of Ce3+ ion. In addition, optically-stimulated luminescence (OSL) signals could be detected in all the crystals when the stimulation wavelength was 470 nm. The OSL dose response functions showed linearly proportional relationship from 10 to 1000 mGy in all the Ce-doped crystals. The thermally-stimulated luminescence (TSL) glow curves exhibit three peaks due to antisite of Al3+ ion, V center and antisite of Mg2+ ion. All the Ce-doped crystals showed improved TSL intensity and dose response sensitivity compared the undoped crystal. The 0.2 and 1% Ce-doped crystals showed linearly response at the dose range of the 0.1–1000 mGy. •We have synthesized MgAl2O4 single crystal doped with Ce by floating zone method.•We have characterized the photoluminescence, scintillation and dosimetric properties.•All samples showed luminescence properties due to some defects and Ce3+ ion.