One of the goals of our research on transition metal alloy nanoparticles is to utilize Computational Chemistry tools to discover the ways to synthesize transition metal alloy nanoparticles with special phase properties as optimal catalysts for reactions of interest, such as oxygen reduction reaction and hydrogenation of coal. In this presentation, I will discuss the results of two alloy nanoparticles, PtAu and PtVFe. I will also present the synergetic results of unraveling PtVFe nanoparticles by coupling computational chemistry with experimental work.