With the increasing levels of anthropogenic carbon dioxide emissions, the need for climate change mitigation has never been more urgent. Developing mass scalable, efficient, and affordable decarbonization technology is a key objective for this generation of scientists. Existing methods for CO2 removal are facilitated by thermally driven systems and thus suffer from being energy-intensive and inefficient. Joint efforts between computational and experimental chemistry fields can help steer research toward uncovering valuable insight into CO2 reactivity with the ideal sorbent.