Abstract: Covalent organic frameworks(COFs) are a new class of porous crystalline materials connected through covalent bonds. COFs possess the essential advantages such as flexible monomer-monomer linkage type, adjustable structure, abundant active sites, large specific surface area and stable physical and chemical properties.These features have brought it to widespread attention in the fields of gas storage and separations, energy storage, catalysis and optoelectronics. Herein the COFs materials are introduced from the aspects of structure design, synthesis, functionalization, structure analysis/characterization and crystallization control; an overview on the current research in the application of COFs materials for the separation of key nuclides is reviewed; and the development and future research direction of the novel materials in nuclide separation is prospected.