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The continuous development of innovative optical materials with lanthanoid ions as activators has emerged as a modern sector of materials chemistry. The experience with the fabrication of single crystals with the optical float zone has motivated one to investigate the luminescence of Nd3+ and Ho3+ ions in the garnets (Gd3−xREx)In2Ga3O12 (RE = Nd and Ho, x = 0; 0.15–0.30). Upon usage of an Ar/O2 (80:20 ratio) atmosphere and application of an auxiliary pressure (6 bar) to suppress In2O3 evaporation, single‐crystalline domain sizes in the order of ≈6 × 6 × 1 mm3 are obtained. Structural analysis confirms the formation of a cubic garnet phase with space group Ia3¯d $I a \\bar{3} d$ , with the substituents incorporated in accordance with Vegard's law. Backscattered electron imaging and energy‐dispersive X‐ray spectroscopy are conducted, demonstrating a homogeneous elemental distribution within the crystals. Photoluminescence studies are carried out, revealing the characteristic narrow‐line 4f n → 4f n transitions of Nd3+ and Ho3+, with decay times in the submillisecond range, suggesting non‐negligible cross‐relaxation effects are present. Despite this, the large nearest‐neighbor Gd–Gd distance (3.88 Å) in Gd3In2Ga3O12 and the low phonon cutoff energy (≈700 cm−1) are found to limit cross‐relaxation pathways, preserving significant photoluminescence brightness. These results highlight the potential of Gd3In2Ga3O12:RE3+ single crystals as promising candidates for advanced optical applications. Nd3+‐ and Ho3+‐doped Gd3In2Ga3O12 single crystals have been successfully synthesized via the optical float zone method. Their structure and optical characterization demonstrate efficient narrow‐line 4f–4f emission, low cross‐relaxation, and bright photoluminescence, indicating their potential as advanced optical materials for photonic applications.