Here, we describe a templating approach to circumvent these challenges and install well-defined binuclear metal active sites in framework pores, irrespective of the active site density (Fig. ). Thermolabile tertiary carbamate crosslinkers are used to tether pairs of amine functional groups during framework synthesis. Postsynthetic crosslinker cleavage reveals templated aryl-and alkylamines that can be used to graft atomically precise bimetallic iminopyridine and bis(2-pyridylmethyl)amine complexes with a variety of metals (e.g., Mn(II), Fe(II), Co(II), Ni(II), Cu(I), and Cu(II)). The structural integrity of the frameworks is confirmed by powder X-ray diffraction and gas sorption measurements, while the local structure of the metal centers is probed by density functional theory (DFT), extended X-ray absorption fine structure (EXAFS) spectroscopy, and electron paramagnetic resonance (EPR) spectroscopy.