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Almost 20 years ago, the first CO₂ capture and storage (CCS) project began injecting CO₂ into a deep geological formation in an offshore aquifer. Relevant science has advanced in areas such as chemical engineering, geophysics, and social psychology. Governments have generously funded demonstrations. As a result, a handful of industrial-scale CCS projects are currently injecting about 15 megatons of CO₂ underground annually that contribute to climate change mitigation. However, CCS is struggling to gain a foothold in the set of options for dealing with climate change. This review explores why and discusses critical conditions for CCS to emerge as a viable mitigation option. Explanations for this struggle include the absence of government action on climate change, economic crisis–induced low carbon prices, public skepticism, increasing costs, and advances in other options including renewables and shale …