In this work we demonstrate that the tuning the of relative strength of the ligand field of the MOF linkers and adsorbate can result in a near-room temperature spin crossoverassisted gas release. Due to the exceptional tunability of their composition and the large number of already existing MOFs, one can expect that recent developments on statistical methods applied to materials science can allow for the discovery of specific frameworks for this strategy for possibly any adsorbate molecule of choice. Therefore, we are confident that the understanding provided here will assist future computational and synthetic efforts towards the development of a novel mechanism yielding a large change in gas affinity for energy-efficient gas capture and/or H2 storage technologies.