In addition to discovering a new MOF Ni(PyC-m-NH 2 ) 2 for Xe/Kr separations-which could be useful for the industrial recovery of Xe and Kr from air separation units, capturing Xe and Kr from off-gases of spent nuclear fuel reprocessing, or detecting illicit nuclear weapons tests-our study illustrates the computation-informed optimization of the chemistry of a "lead" MOF for an adsorption task. In the future, models and algorithms will be able to automatically orchestrate autonomous, robotic platforms to tune the chemistry of MOFs for their various adsorption-based applications .