Iminopyridine formation and metalation in MOFs has been previously demonstrated by several groups, and both stepwise and one-pot synthetic approaches have been explored. In the stepwise approach, excess 2-pyridinecarboxaldehyde (PyCHO) is first added to the amine-functionalized framework to form discrete MOF-supported iminopyridine sites, which are subsequently metalated in a second step. In the one-pot approach, excess PyCHO and metal halide salt (e.g., NiCl2) are combined together to form a molecular (PyCHO)MX2 complex, which is then combined with the framework to form the desired metalated iminopyridine species. We first tested the one-pot condensation and metalation of 1-NH2 with 10 equiv of 2pyridinecarboxaldehyde and metal salt (NiCl2 or CuCl) in methanol. Excitingly, we observed nearquantitative conversion of 1-NH2 to 1-(IP)M (M = NiCl2, CuCl), a framework containing surface-supported bimetallic metal iminopyridine complexes (90% yield for NiCl2 and 100% for CuCl) (Table , Table ). Successful iminopyridine formation and metalation were quantified by 1 H NMR and ICP analysis of digested frameworks, respectively (Table ). Both crystallinity and surface area were maintained in the metalated frameworks (Fig. ), and a BET surface area of 1700 m 2 /g was observed for 1-(IP)CuCl (Fig. ).