In this paper, three of the leading options for large scale CO2 capture are reviewed from a technical perspective. We consider solvent-based chemisorption techniques, carbonate looping technology, and the so-called oxyfuel process. For each technology option, we give an overview of the technology, listing advantages and disadvantages. Subsequently, a discussion of the level of technological maturity is presented, and we conclude by identifying current gaps in knowledge and suggest areas with significant scope for future work. We then discuss the suitability of using ionic liquids as novel, environmentally benign solvents with which to capture CO2. In addition, we consider alternatives to simply sequestering CO2—we present a discussion on the possibility of recycling captured CO2 and exploiting it as a C1 building block for the sustainable manufacture of polymers, fine chemicals, and liquid fuels. Finally, we present a discussion of relevant systems engineering methodologies in carbon capture system design.