A lot of research has been focused on finding the optimal MOF for carbon capture. Ideally, one would like to have a set of experimental pure components and mixture isotherms to test the approach we developed here. However, the number of MOF structures for which accurate mixture adsorption isotherms have been experimentally measured over a large range of pressures, temperatures, and compositions is very limited, especially for a mixture of CO 2 and N 2 . Therefore, we rely on molecular simulations to predict the adsorption isotherms of both, the pure components and their mixture. Here, we use a set of 500 MOF structures that were chosen to represent a diverse set of metals, linkers, ligands, pore sizes, and topologies. In our molecular simulations, we assumed that the crystal structures are rigid. First, each crystal structure was cleaned (i.e., atomic overlaps were removed, solvent molecules were removed, and missing hydrogen atoms have been added) and subjected to Density functional theory (DFT) geometry optimization. The DFT electronic density was also used to compute partial charges via the DDEC protocol. The TraPPE 32 force-field was used to describe the CO 2 -CO 2 , N 2 -N 2 and CO 2 -N 2 interactions, whereas for the guest-MOF interactions the TraPPE-UFF 33 force-field combination was the selected one, as these are common force fields adopted by the community.