Adsorptive separation has been widely used in petroleum, chemical, pharmaceutical, environmental protection and many other fields due to the advantages of high efficiency and low-energy consumption. Therein, the structural characteristics (such as specific surface area, pore size, pore volume, surface functional groups, etc.) of the adsorbent are the key factors that affect the adsorption capacity and separation efficiency. Metal-organic framework (MOF) materials have excellent pore structures and abundant functional groups (—NH₂, —CHO, etc.), which can be easily post-modified and functionalized with specific functions, thus enhancing the interaction between MOFs and adsorbates and achieving high adsorption capacity and separation selectivity. In this context, the synthesis strategies of MOF-NH₂/CHO materials were firstly outlined, then the research progress of imine covalently post-modified MOF (ICPSM-MOF) materials was summarized, and their applications in gas and liquid adsorption separation were emphasized. In addition, the difficulties and challenges faced by the current ICPSM-MOFs were finally analyzed, and the future research trend of ICPSM-MOFs was also put forward.