Plasmonic nanostructures with tunable optical properties and their designed spatial arrangements can facilitate a variety of application ranging from plasmonics to biosensors with unprecedented sensitivity. Here we describe a facile and versatile method for fabricating tunable plasmonic substrates based on the reshaping of metal nanocrystals. Anisotropic etching and redeposition of Ag atoms mediated by halide ions transformed Ag nanoprisms deposited on two- or three-dimensional surfaces or in solution into nanostructures with an oblate spheroidal shape, and corresponding localized surface plasmon resonances features could be tuned. The reshaping nanocrystal strategy can even facilitate the preparation of new classes of plasmonic substrates with gradient or patterned plasmonic properties, which cannot be realized easily using existing lithographic techniques. The substrates with gradient plasmonic properties can serve as platforms for tunable surface-enhanced Raman scattering.