Nanoparticles are a mainstay of heterogeneous catalysis. This is in part due to their mesoscopic structure; they can be grown to have large available surface areas which can be both regenerative and durable in reaction. Their utility is possible by the alloys used in their production—however, analysis of their operation is generally at the DFT or molecular dynamics level. This review will present an overview of the post-DFT methods relevant to materials supporting the ORR and OER reactions. Pt-bearing alloys will then be highlighted with a focus on their application in heterogeneous catalysis and the ORR/OER reactions. The current computational approaches to accurately predicting the band properties of the alloys will then be discussed and both the fundamental and applied importance of this modelling will be highlighted.