Recent research on adsorbents is focused on improving CO2 uptake and adsorption kinetics, enhancing dimensional stability and reusability, as well as overcoming moisture sensitivity (for zeolites and MOFs). Optimizing adsorbents for CO2 uptake and selectivity does not necessarily guarantee their applicability in real applications. Design of temperature-swing (favorable for post-combustion capture) or pressure-swing (favorable for pre-combustion capture) adsorption-desorption cycles, as well as different reactor configurations, all pose specific performance and stability requirements on adsorbents and can induce uncertainties in the practical success of an adsorbent that performed well in the lab. More sophisticated modeling to efficiently screen the numerous possible structures (particularly for MOFs) and to predict their performance under complex processing conditions is needed to increase the industrial application potential of CO2 adsorption.