We have designed a strategy for postsynthesis installation of the beta-diketiminate (NacNac) functionality in a metal organic framework (MOF) of UiO-topology. Metalation of the NacNac-MOF (I) with earth abundant metal salts afforded the desired MOF-supported NacNac-M complexes (M = Fe, Cu, and Co) with coordination environments established by detailed EXAFS studies. The NacNac-Fe-MOF catalyst, I center dot Fe(Me), efficiently catalyzed the challenging intramolecular sp(3) C-H amination of a series of alkyl azides to afford a-substituted pyrrolidines. The NacNac-Cu-MOF catalyst, I center dot Cu(THF), was effective in promoting the intermolecular sp(3) C-H amination of cyclohexene using unprotected anilines to provide access to secondary amines in excellent selectivity. Finally, the NacNac-Co-MOF catalyst, I center dot Co(H), was used to catalyze alkene hydrogenation with turnover numbers (TONS) as high as 700 000. All of the NacNac-M-MOF catalysts were more effective than their analogous homogeneous catalysts and could be recycled and reused without a noticeable decrease in yield. The NacNac-MOFs thus provide a novel platform for engineering recyclable earth abundant -element-based single-site solid catalysts for many important organic transformations.