The development of new microporous materials for adsorption separation processes is a rapidly growing field because of potential applications such as carbon capture and sequestration (CCS) and purification of clean‐burning natural gas. In particular, new metal‐organic frameworks (MOFs) and other porous coordination polymers are being generated at a rapid and growing pace. Herein, we address the question of how this large number of materials can be quickly evaluated for their practical application in carbon dioxide separation processes. Five adsorbent evaluation criteria from the chemical engineering literature are described and used to assess over 40 MOFs for their potential in CO2 separation processes for natural gas purification, landfill gas separation, and capture of CO2 from power‐plant flue gas. Comparisons with other materials such as zeolites are made, and the relationships between MOF properties and CO2 separation potential are investigated from the large data set. In addition, strategies for tailoring and designing MOFs to enhance CO2 adsorption are briefly reviewed. Looking for holes: How can new microporous materials, such as metal–organic frameworks (MOFs, see picture), be quickly evaluated for their practical application in CO2 separation processes? Five adsorbent evaluation criteria are used to assess over 40 MOFs for their potential in natural gas purification, landfill gas separation, and capture of CO2 from power‐plant flue gas. Comparisons with other materials such as zeolites are made.