Based on the solidification heat transfer model and the CAFE model, the solidification behavior and structure of 2311 die steel, with a cross-section dimension of 415 × 2270 mm at different casting speeds, specific water flow and superheat, is numerically simulated. Nail-shooting and acid-etching experiments are carried out on the slab to verify the model’s macroscopic size. With the increase in casting speed, the slab’s central equiaxed grain ratio (ECR) decreases and the average grain size increases. The increase in superheat promotes the growth of columnar grains and inhibits the growth of central equiaxed grains. When the superheat increases from 23 to 38 K, the ECR decreases from 43.2 to 29.64%, and the average radius of grains increases from 0.89 to 1.01 mm. With the increase in specific water flow, the ECR decreases, and the average grain radius is the smallest when the specific water content is 0.32 L kg−1. Finally, the slab quality is improved by process optimization, and the central segregation index of carbon decreases from mean value of 1.15 to 1.05.