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We report a surface-enhanced Raman scattering (SERS) substrate with plasmon resonances at both excitation and Stokes frequencies. This multilayer structure combines localized surface plasmons on the nanoparticles with surface plasmon polaritons excited on a gold film. The largest SERS enhancement factor for a gold device is measured to be 7.2 × 10⁷, which is more than 2 orders of magnitude larger than that measured on a gold nanoparticle array on a glass substrate. The largest SERS enhancement for a silver device is measured to be 8.4 × 10⁸.