In this paper, the self-Q-switched solid-state laser crystal Cr 4+,Nd 3+:Gd 3Ga 5O 12 (Cr,Nd:GGG) has been grown by the Czochralski method. The absorption spectra properties of this crystal in different parts are reported. The growth parameters and energy level of Cr 4+ ions were studied; in the absorption spectra there are two absorption bands at 808 and 881 nm, respectively, which are suitable for GaAlAs diode laser pumping, and there is an absorption band around 1060 nm, which is suitable for self-Q-switched laser. The presence of Cr 4+ ions in Cr,Nd:GGG single crystals are confirmed by measuring the fluorescence spectrum of Cr 4+ ions when pumped at 940 nm. These crystals are potential materials for compact, efficient, high stability diode-laser-pumped passive Q-switched solid-state laser.