Tb3Ga5O12 (TGG) single crystals have excellent optical isolator characteristics.However, TGG single crystals grown by the Czochralski method sometimes contain radial stripes along the growth direction, which degrade their optical isolator characteristics.These radial stripes may be caused by a composition mismatch between the melt and crystals.In this study, we grew 25 mmϕ TGG single crystals from Tb-rich melts and precisely measured their lattice constantsThe relationship between the composition and lattice constants was determined using sintered polycrystalline TGG.Based on these experiments, the congruent-melting composition was found to be 37.9 mol% Tb2O3.High-quality, 50-mmϕ TGG single crystals without radial stripes were grown using a starting material composition of 37.8 mol% Tb2O3, considering the evaporation of Ga2O3 from the melt during crystal growth.We repeatedly grew TGG single crystals by adding the TGG starting material to the residue in the crucible used for growth to complete four addnl. growth processes.The fluctuation of in the lattice constant of the TGG boules for the first and fifth growths was within 0.0002 Å, which corresponds to a Tb2O3 composition uniformity of 0.01 mol% Tb2O3.Therefore, we have succeeded in growing uniform TGG single crystals industrially with composition fluctuations within only 0.01 mol% by optimizing the composition of the TGG starting material to 37.8 mol% Tb2O3.