Ce3+ and Dy3+ co-doped Y3Al5O12 (abbr. as Ce, Dy: YAG) single crystal was grown by the Czochralski method. As compared with the absorption spectrum of Dy: YAG crystal, the synchronous doping of Ce3+ ions into Dy: YAG crystal resulted in a wide excitation band in the 425–500 nm region peaking around 447 nm owing to the 4f→5d transition of Ce3+ ions, and inhomogeneous broadening absorption with the full width at half maximum (FWHM) from 4 nm to 39 nm. Furthermore, due to the efficient energy transfer from Ce3+ to Dy3+ ions in YAG crystal, under 447 nm excitation Ce, Dy: YAG crystal showed intense and wide characteristic yellow green emission, whose intensity increased by 12.3 times and FWHM from 12 nm to 113 nm as compared with Dy: YAG crystal. The fluorescence lifetime of Dy3+: 4F9/2 level has increased from 693.1 μs to 2.062 ms. Based on the above results, Ce, Dy: YAG crystal would be an excellent candidate for the realization of yellow green waveband laser output.