Concentrations of carbon monoxide in rainwater collected at widely diverse locations show up to a 200-fold supersaturation relative to the partial pressure of the gas in the atmosphere. These results indicate the existence of an additional natural source of carbon monoxide not heretofore considered. Production of carbon monoxide in clouds is tentatively attributed to the photochemical oxidation of organic matter or the slight dissociation of carbon dioxide induced by electrical discharges, or both. Methane concentrations measured in the same rainwater show that the partitioning of this gas, unlike that of carbon monoxide, is very close to a state of equilibrium.