ABSTRACT Various Ni‐based metalloenzymes employ synergistic heterometallic cooperativity where a Ni center and a second metal ion cofacilitate small‐molecule conversion. Inspired by these biological systems, synthetic model complexes have been developed that exploit bimetallic cooperativity to achieve analogous reactivity. In this work, we report a bimetallic Ni−Zn complex comprising a pincer‐type diamido‐diaminodiphosphine ligand, in which a weakly Lewis acidic Zn(II) center stabilizes a T‐shap