Combining information from time-resolved X-ray and neutron scattering with theoretical calculations has revealed the elegant mechanism whereby hydrogen crystalline silicotitanate (H-CST; H2Ti2SiO7 center dot 1.5H(2)O) achieves its remarkable ion-exchange selectivity for cesium. Rather than a simple ion-for-ion displacement reaction into favorable sites, which has been suggested by static structural studies of ion-exchanged variants of CST, Cs+ exchange proceeds via a two-step process mediated by conformational changes in the framework. Similar to the case of ion channels in proteins, occupancy of the most favorable site does not occur until the first lever, cooperative repulsive interactions between water and the initial Cs-exchange site, repels a hydrogen lever on the silicotitanate framework. Here we show that these interactions induce a subtle conformational rearrangement in CST that unlocks the preferred Cs site and increases the overall capacity and selectivity for ion exchange.