Surface-enhanced Raman spectroscopy (SERS) is highly dependent upon the substrate, where excitation of the localized metal surface plasmon resonance enhances the vibrational scattering signal of proximate analyte molecules. This article reviews recent progress in the fabrication of SERS substrates and the requirements for characterization of plasmonic materials as SERS platforms. We discuss bottom-up fabrication of SERS substrates and illustrate the advantages of rational control of metallic nanoparticle synthesis and assembly for hot spot creation. We also detail top-down methods, including nanosphere lithography for the preparation of tunable, highly sensitive, and robust substrates, as well as the unique benefits of tip-enhanced Raman spectroscopy for simultaneous acquisition of molecular vibrational information and high spatial resolution imaging. Finally, we discuss future prospects and challenges in SERS, including the development of surface-enhanced femtosecond stimulated Raman spectroscopy, microfluidics with SERS, creating highly reproducible substrates, and the need for reliable characterization of substrates.