Bimetallic nanoparticles (NPs) are complex systems with properties that far exceed those of the individual constituents. In particular, association of a noble metal and a first-row transition metal are attracting increasing interest for applications in catalysis, electrocatalysis, and magnetism, among others. Such objects display a rich structural chemistry thanks to their ability to form intermetallic phases, random alloys, or core-shell species. However, under reaction conditions, the surface of these nanostructures may be modified due to migration, segregation, or isolation of single atoms, leading to the formation of original structures with enhanced catalytic activity. In this respect, Zakhtser et al. report in this issue of ACS Nano the synthesis and study of the chemical evolution of the surface of a series of PtZn nanostructured alloys. In this Perspective, we report some selected examples of bimetallic nanocatalysts and their increased activity compared to the corresponding pure noble metal, with a special focus on Pt-based systems. We also discuss the mobility of the species present on the catalyst surface and the electronic influence of one metal to the other. Bimetallic nanocrystals, which comprise a noble metal (in particular, a platinum group metal) and a non-noble metal (in general, a first-row transition metal), are attracting a lot of interest because of