Improving the separation efficiency of the layer melt crystallization process is a key but difficult task. Herein, a comprehensive model involving both crystallization and sweating was proposed and used to optimize the operating time of crystallization and sweating processes. The crystallization process was modeled based on the relationship between differential and integral distribution coefficients under a constant layer growth rate. For the sweating process, an empirical sweating equation was employed to govern the sweating model, the parameters of which were determined experimentally using P-xylene as the model substance. The separation efficiency was then optimized by minimizing the operating time at a given product purity and yield. A sensitivity analysis showed that the crystallization and sweating times nonlinearly increase with increasing yield. After the yield exceeds 0.65, an increasing crystallization time is the dominant factor in improving the separation efficiency, while the sweating time and ratio even slightly decrease. The total operating time at low yield is U-shaped with the layer growth rate. The optimal layer growth rate decreases with increasing yield. This model provides guidance for determining the optimal operating parameters of layer melt crystallization and sweating processes.