This chapter reviews the published work to date on the interaction of CO2 and CO with frustrated Lewis pairs (FLPs). The ability of FLP-derived systems reversibly to bind and release CO2 is a dramatic and exciting development, offering new routes to sequester this environmentally important molecule. Furthermore, in combination with FLPs' documented ability to cleave H2 heterolytically, new CO2 hydrogenation chemistry has been uncovered. Novel tandem catalytic processes involving FLPs are beginning to be developed which allow the chemical functionalisation of CO2. Structure-function relationships which affect the thermal stability of FLP-CO2 adducts are highlighted, alongside an insight towards the future design of successful FLP-mediated CO2 hydrogenation catalysts.