Metal-organic frameworks are a class of organic-inorganic hybrid and crystalline materials based on coordinatively bonded porous network. But the structure and function have been seldom investigated. The effective processing of MOF devices have always been hindered by the intrinsic feature of crystalline powders. The utilization of thermal rheology of glass material is expected to realize the effective preparation of grain-boundary-free and isotropic MOF glass membrane, which is one of the key goals of porous chemistry in the future. Different types of MOF glasses have been prepared by covering melt-quenching, mechanical or pressure treatment, bottom-up assembly in solution, ionic liquid-assisted melting and sequential perturbation. Nevertheless, the crystallization behavior of liquid and supercooled liquid greatly affects the processing and mechanical, optical, and electrical properties of glass materials, but the mechanism of microstructure evolution during the crystallization process is far from clear. It’s even less clear on systematic study of the crystallization and high-temperature dynamic coordination chemistry for new MOF glass.