The tBuPONOP (2,6-bis(di-tert-butyl-phosphinito)pyridine) complexes of iron and cobalt, (tBuPONOP)FeCl2 (1) and (tBuPONOP)CoCl2 (2)) have been prepared. Both complexes are paramagnetic and the solid-state structures of 1 and 2 were determined by single crystal X-ray diffraction studies. Analogous Fe and Co complexes of the tBuPNP (2,6-bis(di-tert-butyl-phosphinomethyl)pyridine) ligand (3 and 4, respectively) were prepared to allow comparison between the closely related pincer ligands in the hydrosilylation of carbonyl moieties. All four complexes were found to be catalytically active when treated with NaBEt3H, which was assumed to generate a metal-hydride species in-situ.