This feature article covers a long-term project in our laboratory at the University of Saskatchewan towards the rational synthesis of controlled-architectures of gold-palladium bimetallic nanoparticle catalysts for use as low-temperature alcohol oxidation catalysts. Syntheses involve controlled growth of nanoparticle architectures via solution-based nanoparticle synthetic strategies, followed by deposition of the designed particles onto solid supports. In addition, characterization methods used to elucidate structures of the synthesized particles before and after activation for catalysis will be discussed. This includes traditional characterization methods such as transmission electron microscopy and X-ray absorption fine structure spectroscopy (EXAFS), but also includes, more recently, the use of in situ X-ray absorption spectroscopy studies of gold-palladium nanoparticle catalysts. Strategies and challenges towards the rational synthesis of heterogeneous supported-nanoparticle catalysts based on bimetallic nanoparticle precursors will be detailed and contrasted with more traditional routes to synthesize such catalytic materials.