In outer space, high-energy irradiation of cryogenic ice mixtures of abundant water and carbon dioxide is expected to form solid carbonic acid, Experiments and thermodynamic analyses show that crystalline carbonic acid sublimates without decomposition. Free-energy considerations based on highly accurate molecular quantum mechanics, in combination With vapor pressures resulting from experimental sublimation rates, suggest that in the gas phase, a monomer and dimer of carbonic acid are in equilibrium, comparable to that of formic acid. Gaseous carbonic acid could be present in comets, an Mars and outer solar system bodies, in interstellar icy grains, and in Earth＇s upper atmosphere.