We conclude that the materials at the top of the diffusion-enabled MOF ranking are high-performing CO 2 sorbents with the potential to challenge, or even surpass, the performance of the best solid sorbents deployed today. For enabling their validation and exploration, we have made our data publicly available, see Data availability. The computational simulation workflow for molecular diffusivity, which is based on Crystallographic Information File (CIF) format and made available as open-source code base, see Code availability, could be similarly applied to the evaluation of broader classes of solid sorbents, including covalent organic frameworks and zeolites.