We report catalytic silylation of dinitrogen to tris(trimethylsilyl)amine by a series of trinuclear first row transition metal complexes (M = Cr, Mn, Fe, Co, Ni) housed in our tris(β‐diketiminate) cyclophane (L3–). Yields are expectedly dependent on metal ion type ranging from 14 to 199 equiv. NH4+/complex after protonolysis for the Mn to Co congeners, respectively. For the series of complexes, the observed trend for the number of turnovers as a function of metal ion type is Co > Fe > Cr > Ni > Mn, consistent with prior reports of greater efficacy of Co over Fe in other ligand systems for this reaction.