Persistent phosphor Gd3Al2Ga3O12:Ce3+-Cr3+ (GAGG:Ce3+-Cr3+) has been synthesized by solution combustion synthesis (SCS) incorporating mixed organic fuels of glycine and urea at 773 K. Using only single fuel can lead to incomplete combustion and amorphous products. Without additional heat treatment, a porous and pulverized GAGG:Ce3+-Cr3+ powders can be obtained when the fuel ratio ϕ = 1. The products exhibited yellow color emission in visible light photoluminescence. This emission is originated from Ce3+. Photoluminescence excitation spectra indicated that GAGG:Ce3+-Cr3+ can be well excited by blue light, marking its potential for white LED lights application. In comparison with green luminescence Y3Al2Ga3O12 doped with Ce3+-Cr3+ (YAGG:Ce3+-Cr3+), the yellow color in GAGG:Ce3+-Cr3+ is due to crystal field splitting when Y is substituted by Gd. Also, electron energy-loss spectroscopy measurement using scanning electron microscopy (STEM-EELS) showed that the band gap decreased in 6.14 eV, 6.05 eV and 5.93 eV order when Ga content (x = 2.5, 3, 3.5) increased. The bandgap change showed that the trap level produced by Cr3+ ions affected the persistent luminescence. In this study, when Ga content x = 3, Gd3Al5-xGaxO12:Ce3+-Cr3+ exhibited the longest persistent luminescence.