In the wake of sustainable development, materials research is going through a green revolution that is putting energy-efficient and environmentally friendly materials and methods in the limelight. In this quest for greener alternatives, covalent organic frameworks (COFs) have emerged as a new generation of designable crystalline porous polymers for a wide array of clean-energy and environmental applications. In this contribution, we categorically review the merits and shortcomings of COF bulk powders, nanosheets, freestanding thin films/membranes, and membranes on porous supports in various separation processes, including separation of gases, pervaporation, organic solvent nanofiltration, water purification, radionuclide sequestration, and chiral separations, with particular reference to COF material pore size, host–guest interactions, stability, selectivity, and permeability. This review covers the fabrication strategies of nanosheets, films, and membranes, as well as performance parameters, and provides an overview of the separation landscape with COFs in relation to other porous polymers, while seeking to interpret the future research opportunities in this field.

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