Since the time of the industrial revolution, the atmospheric CO2 concentration has risen by nearly 35 % to its current level of 383 ppm. The increased carbon dioxide concentration in the atmosphere has been suggested to be a leading contributor to global climate change. To slow the increase, reductions in anthropogenic CO2 emissions are necessary. Large emission point sources, such as fossil-fuel-based power generation facilities, are the first targets for these reductions. A benchmark, mature technology for the separation of dilute CO2 from gas streams is via absorption with aqueous amines. However, the use of solid adsorbents is now being widely considered as an alternative, potentially less-energy-intensive separation technology. This Review describes the CO2 adsorption behavior of several different classes of solid carbon dioxide adsorbents, including zeolites, activated carbons, calcium oxides, hydrotalcites, organic–inorganic hybrids, and metal-organic frameworks. These adsorbents are evaluated in terms of their equilibrium CO2 capacities as well as other important parameters such as adsorption–desorption kinetics, operating windows, stability, and regenerability. The scope of currently available CO2 adsorbents and their critical properties that will ultimately affect their incorporation into large-scale separation processes is presented.