During the first two close flybys of the moon Enceladus in 2005, Cassini discovered a deflection in the local magnetic field that is characteristic for the existence of a thin but significant atmosphere. Other measurements obtained at that time point to ionized water vapor as its main constituent. Cassini also observed water ice geysers erupting from the south pole of Enceladus, which gives more credibility to the idea that Enceladus is supplying the particles of Saturn's E ring. Mission scientists began to suspect that there may be pockets of liquid water near the surface of the moon that fuel the eruptions.

On March 12, 2008, Cassini made a close fly-by of Enceladus, passing within 50 km of the moon's surface. The spacecraft passed through the plumes extending from its southern geysers, detecting water, carbon dioxide and various hydrocarbons with its mass spectrometer, while also mapping surface features that are at much higher temperature than their surroundings with the infrared spectrometer. Cassini was unable to collect data with its cosmic dust analyzer due to an unknown software malfunction.

On April 3, 2014, nearly ten years after Cassini entered Saturn's orbit, NASA reported evidence of a large salty internal ocean of liquid water in Enceladus. The presence of an internal salty ocean in contact with the moon's rocky core, places Enceladus "among the most likely places in the Solar System to host alien microbial life" . On June 30, 2014, NASA celebrated ten years of Cassini exploring Saturn and its moons, highlighting the discovery of water activity on Enceladus among other findings.