Limiting carbon output is indeed one route to a sustainable future, but in parallel, what if the waste carbons could be efficiently recaptured and effectively recycled—i.e., flipping carbon from a waste to a resource? Unlike separating plastic containers from a bin, extracting gaseous carbon dioxide and monoxide (among other products) from the atmosphere is a large-scale problem that requires molecular solutions. Herein, Jeff Reimer discusses the challenges, opportunities, and emerging material technologies for carbon capture.