There is a consensus about a long-term goal of a carbon-neutral energy cycle, but the CO2 emissions to the atmosphere are currently very large. Carbon Capture and Storage (CCS) technologies could allow a transformation of the global energy system into a carbon-neutral one and simultaneously keeping the temperature rises within agreed bounds. The CO2 separation step of CCS is, however, very expensive, and adsorption-driven technologies have been put forward as alternatives. Hence, a recent focus has been on studying solid adsorbents for CO2, which include activated carbons, zeolites, metal-organic frameworks, and amine-modified silica. In this context, we summarize the literature concerning CO2 sorption studied with Nuclear Magnetic Resonance (NMR), outline selected NMR methods, and present an outlook for further studies.