Surface-enhanced Raman spectroscopy (SERS) is a popular and potential area of investigation in many applications because of its high sensitivity even at mono-molecular level. SERS substrates that typically composed of metal nanostructures can enhance the Raman signal level up to several orders of magnitude, making it a powerful analytical tool in chemical and biomedical applications. The present book chapter is aimed to provide insight about design and latest developments on metal nanoparticles and their application in the field of SERS. The chapter starts with the discussion of basic concept and theories of Raman scattering and SERS based on examples from recent research. It then primarily reviews various potential metallic nanostructures and their geometry as SERS substrates, followed by recent reports and theories on application of bimetallic nanostructures for the purpose. Toward the end, we briefly discuss the research progress in designing hybrid SERS substrates using emerging materials like photonic crystals and graphene.