In the quest for earth-abundant catalyst alternatives for hydrogen electrolyzers and CO2-driven fuel cells, interest in ternary base metal chalcogenide materials has boomed owing to their relatively high abundance and promising activities. However, further improvements are needed to achieve competitive performance for widespread application. Tuning the activity of ternary base metal chalcogenides is a challenging, multifactorial problem because of the wide range of constituent elements (base metal, chalcogenide, and additives) that can be employed as well as the impact of catalyst morphology and crystallinity on reactivity. We are developing atomically precise, molecular variants of these catalysts that exhibit active site tunability and functionality. These multimetallic models will allow us to rationally and systematically test hypotheses concerning the cooperative involvement of surface metal and chalcogenide sites in catalysis. Ultimately, we will seek to integrate these catalysts into robust, porous networks for enhanced longevity and function.