The photoluminescence (PL) and scintillation properties of (C 6 H 5 C 2 H 4 NH 3 ) 2 Pb 1−x Cu x Br 4 (x = 0.05, 0.1, 0.25, and 0.5) single crystals prepared by the poor-solvent diffusion method were evaluated. In the PL profiles, free-and bound-exciton luminescence peaks at 410 and 440 nm were observed, respectively. The PL quantum yields (QYs) of the x = 0.05, 0.1, 0.25, and 0.5 samples were 20.0, 19.3, 18.4, and 16.7% with 2% errors, respectively. In the scintillation profiles, a bound-exciton luminescence peak was observed at 440 nm. Under γ-ray exposure with 137 Cs, a photoabsorption peak was observed in all the samples, and the scintillation light yields of the x = 0.05, 0.1, 0.25, and 0.5 samples were estimated to be ~12000, ~11000, ~10000, and ~9700 ph/MeV with 10% errors, respectively.