The understanding of the localized surface plasmons (LSPs) that occur at the geometrically bounded surface of metal nanoparticles continues to advance as new and more complex nanostructures are found. It has been shown that the oscillation of electrons at the metal dielectric interface is strongly dependent on the size, symmetry, and proximity of nanoparticles. Here, we present a new method to chemically control the shape of silver nanocrystals by using a highly anisotropic etching process. Tuning of the etchant strength and reaction conditions allows the preparation of new nanoparticle shapes in high yield and purity, which cannot be synthesized with conventional nanocrystal growth methods. The etching process produces intraparticle gaps, which introduce modified plasmonic characteristics and significant scattering intensity in the near-infrared. These new silver particles serve as excellent substrates for wavelength-tunable, single-particle surface enhanced Raman spectroscopy (spSERS).