Based on the thermal stability analysis by density functional theory and the crystal phase optimization by tolerance factor, the crystal structure was designed. So, a new cubic Ce 3 Sc 2 Ga 3 O 12 (CSGG) garnet material with a high Ce 3+ concentration was synthesized. The centimeter-scale CSGG crystal was grown by the Czochralski method. CSGG exhibits fine magneto-optical properties, which are attributed to the stable valence and high concentration of rare-earth Ce 3+ ions. Compared with commercial Tb 3 Ga 5 O 12 (TGG), CSGG is also paramagnetic, but its magneto-optical properties are better. The Verdet constants of CSGG in 532, 635, 1064, and 1550 nm are −380.0, −258.8, −47.5, and −22.4 rad/T•m, respectively, which are from 1.2 to 2.0 times that of TGG. Moreover, the CSGG crystal has high transmittance in 1500−2300 nm to make up for the poor transmittance of TGG crystal in this band. Also, considering its low raw material cost, the CSGG crystal presents promising application potential. It could be qualified as an essential material for magneto-optical isolators, circulators, and switches within the visible to mid-infrared band.