Ancient Mars had surface liquid water and a dense carbon dioxide (CO2)–rich atmosphere. Such an atmosphere would interact with crustal rocks, potentially leaving a mineralogical record of its presence. We analyzed the composition of an 89-meter stratigraphic section of Gale crater, Mars, using data collected by the Curiosity rover. An iron carbonate mineral, siderite, occurs in abundances of 4.8 to 10.5 weight %, colocated with highly water-soluble salts. We infer that the siderite formed in water-limited conditions, driven by water-rock reactions and evaporation. Comparison with orbital data indicates that similar strata (deposited globally) sequestered the equivalent of 2.6 to 36 millibar of atmospheric CO2. The presence of iron oxyhydroxides in these deposits indicates that a partially closed carbon cycle on ancient Mars returned some previously sequestered CO2 to the atmosphere.