Mononuclear complexes remain the target of the vast majority of catalyst designs. This is part because mechanisms and general principles of dinuclear metal-metal interactions and their impact on catalytic reaction steps remains underdeveloped. My group is playing a major role in the current revival in the use of dinuclear complexes to catalyze reactions with new mechanisms that are faster and more selective compared to traditional mononuclear catalysts. My group’s long-term goals are to discover new mechanisms, reactivity, and selectivity available for two metals compared to one metal and design new dinuclear catalysts and reactions. This has led to collaboration with more than eight experimental research groups around the world. Our recent published works include discoveries of new mechanisms and the origin of reactivity for Ni-Ni catalyzed alkyne cyclotrimerization, Ir-Ta catalyzed alkene hydrogenation, Pd-Ti catalyzed allylic amination, and Rh-Rh catalyzed aziridination and arene C-H amination (ACS Catal. 2017, 7, 4796; Science 2016, 353, 1144; ACS Catal. 2015, 5, 1840; J. Am. Chem. Soc. 2015, 137, 7371; Science 2014, 343, 61). The goals of our current work include development of reactivity and selectivity principles by comparing dinuclear versus mononuclear catalysts and determine the impact of metal-metal pairing. Additionally, we are using calculations to design new dinuclear catalysts for thermal arene borylation and asymmetric reactions.