Mg4Ta2O9 single crystals doped with 0.01, 0.1, and 1% Er were grown using the floating zone method, and their photoluminescence and scintillation properties were studied. X-ray diffraction analysis confirmed that all samples had a hexagonal structure of Mg4Ta2O9. The samples showed that the emission peak at 1550 nm was due to 4f−4f transitions of Er3+ ions, with quantum yields of 32.9, 46.6, and 18.0% for 0.01, 0.1, and 1% doping concentrations, respectively. All samples showed scintillation with a broad emission band at 350 nm due to charge transfer from Ta5+ to O2− ions and emission peak at 1550 nm due to 4f−4f transition of Er3+ ions. The dose rate response functions showed that the detection limit for all samples was 0.06 Gy/h for scintillation detector applications.