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The luminescence, scintillation, and photoconversion properties of the single crystals of Ce3+ doped Tb 3−x Gd x Al 5-y Ga y O 12 (х = 0–1.5; у = 2–2.5) mixed garnets, grown by the micro-pulling-down (μ-PD) method, are investigated as a function of the Tb/Gd ratio with the aim of development of phosphor-convertors of white LED and scintillators. The partial Tb3+ substitution by Gd3+ cations leads to the suitable change of the crystal field splitting of the 5d energy levels of Ce3 ions due to different sizes of the Gd3+ and Tb3+ cations. For this reason, the cation engineering enables to improve the luminescence and scintillation characteristics of Tb 3−x Gd x Al 3-2.5 Ga 2-2.5 O 12 crystals due to increasing the efficiency of Gd3+→ Tb3+→ Ce3+ cascade energy transfer observed in these solid solutions. We have shown that from all the crystals under study, the Tb 3-x Gd x Al 2.5 Ga 2.5 O 12 :Ce (х = 1–1.5) crystal is the best promising candidate for the photoconversion and scintillation applications. • Single crystals of TbGdAGG:Ce grown by the micro-pulling-down method. • Tb3+/Gd3+ ratio control improving the color rendering and scintillation properties. • The best photoconversion properties are shown by Tb 2-1.5 Gd 1-1.5 Al 2.5 Ga 2.5 O 12 :Ce. [ABSTRACT FROM AUTHOR]