The capture of CO2 from the flue gases of stationary industrial sources forms a crucial step to reduce anthropogenic greenhouse gas emissions in the short term. Current technologies based on amine scrubbing require a high regeneration cost and are therefore economically not viable for most CO2 sources. As a result, covalent organic frameworks (COFs), a new class of nanoporous materials with exceptional physicochemical properties, were recently proposed as a promising alternative. To ensure the adoption of COFs for industrial CO2 capture applications, however, it is essential to identify those COFs combining (i) a high stability and crystallinity with (ii) a large CO2 affinity and uptake. To this end, a combined experimental/theoretical approach is pursued here, in which a large database of existing and yet-to-be-synthesized COFs will be constructed and screened. Starting from a COF database, which will be constructed from the building blocks of state-of-the-art COFs for CO2 adsorption and chemical intuition, the materials will be screened both computationally and experimentally for a variety of well-chosen descriptors related to the stability/crystallinity and CO2 capture, after which the best performing COFs are extensively characterized experimentally. This will enable us to design new COF materials outperforming current state-of-the-art technologies for carbon capture in a green and cost-effective way, bringing the long-term ideal of a circular economy closer to reality.