In the following sections, we outline all the elements of the methodology required to assemble material design and multiscale screening workflow in this study, including ML algorithms for predicting adsorption properties, genetic algorithms for generating optimal materials, high fidelity GCMC simulations to validate and refine ML predictions, and process modeling for material performance evaluation. In the Results section, we demonstrate that many designed hypothetical materials, based on experimentally accessible building blocks, exhibit outstanding performance for post-combustion carbon capture, and we explore molecular and structural origins of their performance.