The invention relates to a high-cerium-content scandium-doped gadolinium iron garnet magneto-optical crystal as well as a preparation method and application thereof. The magneto-optical crystal with the chemical formula of Gd3-x-yCexCaySczFe5-z-wVWO 12, is grown by adopting an edge-defined film-fed crystal growth method, wherein x is equal to 0.33-0.54, y is equal to 0.02-0.06, z is equal to 0.45-0.96, and w is equal to 0.01. According to the method, the post-processing technology of the crystal can be simplified, the preparation cost of the crystal is reduced, the crystal growth rate is high,the optical uniformity is good, and the centimeter-scale single crystal can be prepared. By doping a proper amount of Sc, stabilization of an RIG garnet structure is facilitated, unit cells are expanded, the doping amount of Ce in the crystal is increased, the magnetism of the crystal is enhanced, and the high-cerium-content scandium-doped gadolinium iron garnet magneto-optical crystal with goodpermeability, strong magnetism and excellent magneto-optical performance is obtained. The crystal material is expected to be practically applied to devices such as magneto-optical isolators, magneto-optical circulators, magneto-optical modulators and the like.