Appropriate selection of adsorbent materials is essential in developing adsorption-based processes such as CO2 capture. Approximate methods to evaluate material candidates exist using adsorbent evaluation metrics or simplified process models. These approximate methods do not, of course, completely describe the performance of adsorbents in real separation processes. Here, we assess the correlations between approximate predictions and detailed process models of pressure swing adsorption (PSA) at subambient temperatures for postcombustion CO2 capture using metal-organic frameworks (MOFs). Our results indicate that CO2 swing capacity and adsorbent performance score are useful in predicting the ranking of materials for this process. These results illustrate the opportunities and challenges in bridging approximate and detailed methods for evaluating adsorbents for cyclic separations processes.