Abstract. We propose the hypothesis that natural selection, acting on the specificity or preference for CO2 over O2 of the enzyme rubisco (ribulose-1,5-bisphosphate carboxylase/oxygenase), has controlled the CO2:O2 ratio of the atmosphere since the evolution of photosynthesis and has also sustained the Earth's greenhouse-set surface temperature. Rubisco works in partnership with the nitrogen-fixing enzyme nitrogenase to control atmospheric pressure. Together, these two enzymes control global surface temperature and indirectly the pH and oxygenation of the ocean. Thus, the co-evolution of these two enzymes may have produced clement conditions on the Earth's surface, allowing life to be sustained.