Many materials have been explored as potential hydrogen evolution reaction (HER) electrocatalysts to generate clean hydrogen fuel via water electrolysis, but none so far compete with the highly efficient and stable (but cost prohibitive) noble metals. Similarly, noble metals often excel as electrocatalytic counter electrode materials in regenerative liquid-junction photoelectrochemical solar cells, such as quantum dot-sensitized solar cells (QDSSCs) that employ the sulfide/polysulfide redox electrolyte as the hole mediator. Here, we systematically investigate thin films of the earth-abundant pyrite-phase transition metal disulfides (FeS2, CoS2, NiS2, and their alloys) as promising alternative electrocatalysts for both the HER and polysulfide reduction. Their electrocatalytic activity toward the HER is correlated to their composition and morphology. The emergent trends in their performance suggest that cobalt plays an important role in facilitating the HER, with CoS2 exhibiting highest overall performance. Additionally, we demonstrate the high activity of the transition metal pyrites toward polysulfide reduction and highlight the particularly high intrinsic activity of NiS2, which could enable improved QDSSC performance. Furthermore, structural disorder introduced by alloying different transition metal pyrites could increase their areal density of active sites for catalysis, leading to enhanced performance.