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Single crystals of Cs2NaGdBr6 with different Ce+3 activator concentrations were grown by a two-zone Bridgman method. This new compound belongs to a large elpasolite halide (A2BLnX6) family. Many of these elpasolite compounds have shown high luminosity, good energy resolution and excellent proportionality in comparison to traditional scintillators such as CsI and NaI; therefore, they are particularly attractive for gamma-ray spectroscopy applications. This study investigated the scintillator properties of Cs2NaGdBr6:Ce+3 crystals as a new material for radiation detection. Special focus has been placed on the effects of activator concentration (0 to 50 mol.%) on the photoluminescence responses. Results of structural refinement, photoluminescence, radioluminescence, lifetime and proportionality measurements for this new compound are reported.