Pressures up to 0.8 GPa have been used to squeeze a range of sterically “oversized” C5–C8 alkane guest molecules into the cavities of a small-pore Sc-based metal–organic framework. Guest inclusion causes a pronounced reorientation of the aromatic rings of one-third of the terephthalate linkers, which act as “torsion springs”, resulting in a fully reversible change in the local pore structure. The study demonstrates how pressure-induced guest uptake can be used to investigate framework flexibility relevant to “breathing” behavior and to understand the uptake of guest molecules in MOFs relevant to hydrocarbon separation.