DNA origami is ideally suited to arrange plasmonic functional units such as gold and silver nanoparticles with nanometer precision. These nanoparticles can serve as signal-generating or -enhancing elements in optical spectroscopy and chemical and biological sensing, leading to the precise plasmonic assemblies. Additionally, receptors for target molecules can be placed precisely at positions where they trigger the strongest plasmonic response within a specific detection scheme. Building on these possibilities, DNA origami nanostructures have been used as substrates for surface-enhanced Raman scattering and surface-enhanced fluorescence for very efficient detection of molecules in the few- or single-molecule scale. This book chapter provides a short introduction to the optical properties of plasmonic nanoparticles, some procedures to efficiently modify nanoparticles with DNA and an overview over the recent advances and applications in this field.