Ce0.03Gd2.97Ga2Al3O12 (Ce:GGAG) single crystals were successfully grown by the traveling solvent floating zone method (TSFZ). A series of compositions, where the mole ratio is Gd2O3 : Al2O3 = 25 : 75, 27 : 73, 29 : 71, were investigated as solvents. The 25 mol% Gd2O3-75 mol% Al2O3 solvent component was found to be the most effective in stabilizing the molten zone to obtain a crystal rod with uniform diameter. The crystal cracks were relieved clearly due to the improved molten zone stabilization during the crystal growth process. XRD patterns of the obtained crystals prove the garnet structure without any evident second phase. The characteristic Ce3+ emission located at around 540 nm was presented in the photoluminescence and X-ray excited luminescence spectra. The scintillation light yield reaches up to 34 132 pho MeV−1 and scintillation decay time was optimized to 64 ns with a high fast decay component of about 85%. The TSFZ method demonstrated the growth feasibility of Ce:GGAG crystals that have an incongruent-melting trend with lower Ga/Al ratio in the compositions.