Materials capable of selectively adsorbing or releasing water can enable valuable applications ranging from efficient humidity and temperature control to the direct atmospheric capture of potable water. Despite recent progress in employing metal-organic frameworks (MOFs) as privileged water sorbents, developing a readily accessible, water-stable MOF platform that can be systematically modified for high water uptake at low relative humidity remains a significant challenge. We herein report the development of a tunable MOF that efficiently captures atmospheric water (up to 0.78 g water/g MOF) across a range of uptake humidity (27-45%) employing a readily accessible Zn bibenzotriazolate MOF, CFA-1 ([Zn5(OAc)4(bibta)3], H2bibta = 1H,1H'-5,5'-bibenzo[d][1,2,3]triazole), as a base for subsequent diversification. Controlling the metal identity (zinc, nickel) and coordinating nonstructural anion (acetate, chloride) via postsynthetic exchange modulates the relative humidity of uptake, facilitating the use of a single MOF scaffold for a diverse range of potential water sorption applications. We further present a fundamental theory dictating how continuous variation of the pore environment affects the relative humidity of uptake. Exchange of substituents preserves capacity for water sorption, increases hydrolytic stability (with 5.7% loss in working capacity over 450 water adsorption-desorption cycles for the nickel-chloride-rich framework), and enables continuous modulation for the relative humidity of pore condensation. This combination of stability and tunability within a synthetically accessible framework renders Ni-incorporated M5X4bibta3 promising materials for practical water sorption applications.