This article covers cutting-edge research in ionic liquid-based materials and their impact on carbon capture. Ionic liquids boast high thermal stability, low vapor pressure, and great tunability. They can be deployed as either sorbents or supported liquid membranes for carbon capture and other gas separations. Absorption of CO2 in ionic liquids can be achieved via physisorption or chemisorption, depending on the strength of the interaction. For physisorption, both CO2-anion and cation–anion interactions are important factors in dictating CO2 solubility. For chemisorption, the reactivity with CO2 can be tuned by the basicity of the anion while the stability of the ionic liquid can be enhanced by controlling the cation. Marrying ionicity of ionic liquids with porosity leads to novel porous ionic liquids that feature unique properties for facilitating gas transport, while interfacing ionic liquids with microporous membranes allow the ions to gate the pores for selective gas transport. Composite materials of ionic liquids with crystalline materials such as metal–organic frameworks offer scalable heterogeneous interfaces to promote selectivity. Future opportunities include controlling the interaction with CO2 and its transport at the charged or electrified interface with the ionic-liquid electric double layer, as well as combining CO2 capture and conversion with ionic liquids.