We argued that to test the spatial arrangement of a metal on performance, a second inactive metal could be interspersed to create distinct ordered distributions of the metal of interest (Fig. ). But since MOFs are synthesized via reversible reactions to ensure crystallinity, all structural outcomes, including the distribution of multiple metal centers within the framework, are under thermodynamic control. Elegant approaches have been developed that make use of the distinct coordination preferences of two different metal centers to create MOFs in which the two metals occupy separate secondary building units (SBUs), mixed-metal SBUs with defined metal ratios, or ordered sequences . But known approaches based on thermodynamic control can, at most, access one ordered arrangement: if there is an energetically favored ordered arrangement, all alternative ordered arrangements are disfavored. If little or no thermodynamic bias is present, an entropically favored random distribution of metals over lattice sites is obtained . Here we show that a mobility-tuned synthesis approach permits selective synthesis of individual structomers, for which the metal arrangement obtained is controlled by the synthesis procedure. Suites of structomers with distinct arrangements of early-and late-transition metal centers which are commonly used in redox catalysis could thus be obtained. Mobility-tuned synthesis relies on the selection of metal building blocks of distinct sizes (e.g. metal ions, paddlewheels, cages, and groups of cages) that are transformed via a suite of established and reliable reactions .