In summary, we have developed a strategy to precisely template pairs of aryl-and alkylamines in a mesoporous metal-organic framework. The templated amines can be further elaborated to achieve atomically precise bimetallic active sites with tunable ligand environments. The iminopyridine and bis(2pyridylmethyl)amine ligand scaffolds illustrated here have a rich history in organometallic and bioinorganic chemistry, as well as the potential to support unusual bimetallic reactivity. For example, dinucleating iminopyridine ligands have been previously explored in the context of olefin polymerization, while dinucleating polypyridyl scaffolds have been studied for bimetallic O2 activation, anion sensing, and nucleotide hydrolysis. Finally, we note that previous routes to achieve well-defined bimetallic sites in metal-organic frameworks, such as the use of pre-formed clusters containing short metal-metal bonds or geometrically restricted binding pockets, have led to active sites with highly constrained metal-metal distances. Our templated sites, which are conformationally flexible, represent a distinct and complementary alternative to the more rigid, static ligand environments described in earlier reports. Overall, the synthetic precision and flexibility of the templating approach described here will allow researchers to re-examine molecular and enzymatic bimetallic motifs in a heterogeneous context, as well uncover new modes of reactivity.