Metal-organic frameworks (MOFs) are a fascinating class of crystalline nanoporous materials that can be synthesized with a diverse range of pore dimensions, topologies, and chemical functionality. As with other well-known nanoporous materials, such as activated carbon and zeolites, MOFs have potential uses in a range of chemical separation applications because of the possibility of selective adsorption and diffusion of molecules in their pores. We review the current state of knowledge surrounding the possibility of using MOFs in large-scale carbon dioxide separations. There are reasons to be optimistic that MOFs may make useful contributions to this important problem, but there are several critical issues for which only very limited information is available. By identifying these issues, we provide what we hope is a path forward to definitively answering the question posed in our title.