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A series of (Gd, Y, Yb, Tb, Ce)3Al2Ga3O12 compositionally disordered compounds with a garnet structure were prepared in the form of ceramics by sintering in oxygen at 1650 °C for 2 h and studied for the luminescent properties and interaction of ions entering the matrix host. The luminescence features of Ce3+ ions were found to be strongly dependent on the Yb concentration. Photoluminescence and scintillation kinetics are characterized by subnanosecond kinetics when the Yb index in the compound exceeds X = 0.3. It opens an opportunity to create an extremely fast and dense scintillation material emitting in a visible range. A further decrease in the Yb index in the compound leads to an increase in the intensity of Yb3+ infrared (IR) emission, whereas Ce3+ and Tb3+ ions contribute to the luminosity of the material by overlapping intra- and intereconfiguration luminescence bands in the spectral range of 300–700 nm. This finding opens an opportunity to create converter materials tolerant to the corpuscular radiation of isotope sources, providing a high efficiency of electric current production when coupled with a silicon photovoltaic element. The compounds were engineered at the nanoscale level, providing control over electronic excitation transfer between luminescent ions. [ABSTRACT FROM AUTHOR]