Localized surface plasmon resonance (LSPR) excitation in silver and gold nanoparticles produces strong extinction and scattering spectra that in recent years have been used for important sensing and spectroscopy applications. This article describes the fabrication, characterization, and computational electrodynamics of plasmonic materials that take advantage of this concept.Two applications of these plasmonic materials are presented: (1) the development of an ultrasensitive nanoscale optical biosensor based on LSPR wavelength-shift spectroscopy and (2) the use of plasmon-sampled and wavelength-scanned surface-enhanced Raman excitation spectroscopy (SERES) to provide new insight into the electromagnetic-field enhancement mechanism.