Two-neutrino double electron capture is a rare nuclear decay where two electrons are simultaneously captured from the atomic shell. For 124 Xe this process has not yet been observed and its detection would provide a new reference for nuclear matrix element calculations. We have conducted a search for two-neutrino double electron capture from the K-shell of 124 Xe using 7636 kg·d of data from the XENON100 dark matter detector. Using a Bayesian analysis we observed no significant excess above background, leading to a lower 90% credibility limit on the half-life T 1/2 > 6.5×10 20 yr. We have also evaluated the sensitivity of the XENON1T experiment, which is currently being commissioned, and found a sensitivity of T