Carbon dioxide is the main atmospheric greenhouse gas released from industrial point sources. In order to mitigate adverse environmental effects of these emissions, carbon capture, storage, and utilization are required. To this end, several CO2 capture technologies are being developed for application in carbon capture, including aqueous amines and water-lean solvents. Herein we report new aminopyridine solvents with the potential for CO2 capture from coal-fired power plants. These four solvents, 2-picolylamine, 3-picolylamine, 4-picolylamine, and N'-(pyridin-4-ylmethyl)ethane-1,2-diamine, are liquids that rapidly bind CO2 to form crystalline solids at standard room temperature and pressure. These solvents have displayed high CO2 capture capacity (11-20 wt %) and can be regenerated at temperatures in the range of 120-150 degrees C. The advantage of these primary aminopyridine solvents is that a crystalline salt product can be separated, making it possible to regenerate only the CO2-rich solid and ultimately reduce the energy penalty.