We present a high-quality Cr,Nd:YAG crystal with 1.0 at. % Cr3 + and 1.1 at. % Nd3 + grown successfully by the Czochralski method. Spectroscopy results indicate that codoped Cr3 + ions are advantageous for improving pumping efficiency. The maximum average power of 20.24 W operated at 40 Hz and 1.06 μm is obtained on the Cr,Nd:YAG crystal, with electrical-to-optical and slope efficiencies that correspond to 3.00% and 3.77%. Meanwhile, the maximum average power of only 13.32 W is obtained on the Nd:YAG crystal, with the electrical-to-optical and slope efficiencies of 1.97% and 2.47%, respectively. In addition, the laser beam quality of the Cr,Nd:YAG crystal is comparative with that of the Nd:YAG crystal. Therefore, the Cr,Nd:YAG is a promising laser crystal with higher laser performance and stronger radiation-resistant ability than the Nd:YAG crystal. Thus, the Cr,Nd:YAG crystal can be applied to high-power systems and radiant environments.