An off-limb scan of Callisto was conducted by the Galileo near-infrared mapping spectrometer to search for a carbon dioxide atmosphere. Airglow in the carbon dioxide nu(3) band was observed up to 100 kilometers above the surface and indicates the presence of a tenuous carbon dioxide atmosphere with surface pressure of 7.5 x 10(-12) bar and a temperature of about 150 kelvin, close to the surface temperature. A lifetime on the order of 4 years is suggested, based on photoionization and magnetospheric sweeping. Either the atmosphere is transient and was formed recently or some process is currently supplying carbon dioxide to the atmosphere.