Layer melt crystallization has been widely utilized in numerous chemical industries because of its high selectivity for pure products, low energy consumption, and the convenience to industrialization. This review will lay out the research progress and process model development of the key processes (crystal layer growth and impurity distribution) involved in layer melt crystallization. First, the nucleation mechanism, the preparation approaches of the initial crystal layer, and classic experimental configurations are illustrated. Second, modeling approaches are outlined to release the progress of separation effect evaluation, parameter optimization, and sweating process simulation in layer melt crystallization. Novel theories (fractal, porous media, and so on) and technologies (gradient freezing, sonocrystallization, and so forth) with suitable interpretation are potential solutions for the shortcomings of the current process research. Consequently, application areas related to layer melt crystallization are highlighted. Finally, the key issue for further research, challenges, and perspectives will be concluded.