With the negative environmental implications of the anthropogenic emission of greenhouse gases like CO2 having been scientifically established, emphasis is being placed on a concerted global effort to prevent such gases from reaching the atmosphere. Especially important are capture efforts at large point emission sources like fossil fuel power generation, natural gas processing, and various industrial plants. Given the importance and scale of such activities, it is a significant priority to optimize the capture process in terms of speed, energy requirements, and cost efficiency. For CO2 capture, in particular, multiple systems are being pursued both with near-term retrofitting and medium- to long-term designs in mind, including: (1) liquid solvents like amines, carbonates, and ionic liquids (ILs); (2) microporous sorbents like zeolites, activated carbon, and metal-organic frameworks; (3) solid sorbents like metal-oxides and ionic clays; and (4) polymeric and inorganic membrane separators. Each system is unique in its molecular-level guest–host interactions, chemistry, heats of adsorption/desorption, and equilibrium thermodynamic and transport properties as a function of loading, temperature, and pressure. This opens up exciting opportunities for molecular modeling in the design and optimization of materials systems. Here, we offer a brief survey of molecular modeling applications in the field of carbon capture, with a few illustrative examples from our own work primarily involving amine solutions and ILs. Important molecular dynamics, Monte Carlo, and correlations-based work in the literature relevant to CO2 capture in other systems are also discussed. © 2013 Wiley Periodicals, Inc.