The separation of xenon/krypton mixtures is important for both environmental and industrial purposes. The potential of three hydrothermally stable MOFs (MIL-100(Fe), MIL-101(Cr), and UiO-66(Zr)) for use in Xe/Kr separation has been experimentally investigated. From the observed single-component Xe and Kr isotherms, isosteric heat of adsorption (Q(st)(0)), and LAST-predicted Xe/Kr selectivities, we observed that UiO-66(Zr) has the most potential as an adsorbent among the three candidate MOFs. We performed dynamic breakthrough experiments with an adsorption bed filled with UiO-66(Zr) to evaluate further the potential of UiO-66(Zr) for Xe/Kr separation under mixture flow conditions. Remarkably, the experimental breakthrough curves show that UiO-66(Zr) can efficiently separate the Xe/Kr mixture. Furthermore, UiO-66(Zr) maintains most of its Xe and Kr uptake capacity, as well as its crystallinity and internal surface area, even after exposure to gamma radiation (2 kGy) for 7 h and aging for 16 months under ambient conditions. This result indicates that UiO-66(Zr) can be considered to be a potential adsorbent for Xe/Kr mixtures under both ambient and radioactive conditions. (C) 2016 Elsevier B.V. All rights reserved.