A high-performance CO 2 separation membrane consisting of an ion gel has been prepared. The tetra-armed poly(ethylene glycol) ion gel contains a large fraction of ionic liquid (94 wt %) and shows excellent CO 2 permselectivity over a wide temperature range, up to 100°C. We also demonstrate that the ion gel can absorb CO 2 without solvent seeping at a high pressure of 3 MPa.Room-temperature ionic liquids (ILs) have been widely applied to electrochemical, synthetic, and separation processes as green solvents due to their unique properties such as nonvolatility, nonflammability, good thermal stability, and high ionic conductivity. ILs are recognized as designable solvents, and their structural diversity enables us to control their solvent properties, for example, the miscibility with various chemicals such as metal ions, synthesized and biological polymers, and acidic gases. In the last decade, CO 2 absorption and separation technologies using ILs have attracted much attention, because CO 2 is highly soluble in ILs relative to other neutral gases like N 2 , H 2 , and CH 4 . A large number of investigations have been performed until now to improve the CO 2 absorption properties since the first report on the high solubility of CO 2 in the dialkylimidazolium-based IL.1 A membrane separation process generally requires smaller operational energy, lower running cost, and smaller equipment footprint compared with an absorption process. The supported IL membranes (SILMs), i.e., polymeric or inorganic porous materials filled with ILs, show comparable or higher permeabilities and selectivities of CO 2 than conventional polymeric membranes.2 SILMs have a higher long-term stability than supported membranes with organic solvents, because of nonvolatility and high thermal stability of ILs. However, SILMs cannot hold ILs under pressurized conditions, which is a serious disadvantage for the gas separation membrane. Polymeric ILs, i.e., self-crosslinking ILs were also applied as CO 2 separation membranes.3 However, it was pointed out that their separation performances are inferior to those of the SILMs due to the limited CO 2 diffusion in their rigid polymer matrix. Therefore, ion gels with a low polymer content and/or a high fraction of "free" IL content are more favorable materials for CO 2 separation membrane.Recently, some research groups reported the CO 2 separation performances of ion gels with relatively low polymer contents. . They also reported a high-toughness ion gel with 10 wt % triblock copolymer, which was prepared by crosslinking reactions in the IL. 5 The electrical conductivity is about 2/3 that of the neat IL because the ionic mobility is obstructed by the nonconductive part in their ion gel. Kamio et al.4d reported a CO 2 N 2 separation membrane using poly(vinylpyrrolidone)-based ion gels containing 5070 wt % amino acid IL, and the ion gel shows a compression breaking stress of 1 MPa at 70 wt % IL content. They demonstrated that both CO 2 permeability and selectivity are significantly improved with increasing IL ...