Beibei Zhou, Tengwu Zeng, Zhaolin Shi, Gen Zhang, Satoshi Horike, Yue-Biao Zhang,* 
Chem. Asian J. 201914, 3552–3556.
The function of allosteric enzymes can be activated or inhibited through binding of specific effector molecules. Herein, we describe how the skeletal deformation, pore configuration, and ultimately adsorptive behavior of a dynamic metal–organic framework (MOF), (Me2NH2)[In(atp)]2 (in which atp=2‐aminoterephthalate), are controlled by the allocation and orientation of its counter ions triggered by the inclusion/removal of different guest molecules. The power of such allosteric control in MOFs is highlighted through the optimization of the hydrocarbon separation performance by achieving multiple pore configurations but without altering the chemical composition.