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The authors report on the integration of delocalized surface plasmon resonances (SPRs) and localized surface plasmon resonances (LSPRs) on a single device. The submicron SPR device was fabricated with nanoimprint lithography (NIL). Gold nanoparticles for LSPR generation were created and deposited via three methods and analyzed with rhodamine 6 G and surface-enhanced Raman spectroscopy (SERS). Compared to drop-cast and thin film annealing methods, gold nanoparticles fabricated from a diblock-copolymer NIL template produced the most significant effect on the charge-transfer component of the SERS enhancement mechanism due to near-field interactions at the 10 nm inter-particle separation region. The authors also report a 26% enhancement of optical resonance with an integrated SPR-LSPR plasmonic device consisting of a two-dimensional submicron aluminum grating fully coupled with gold nanoparticles measuring 20.4 nm in diameter in a water medium. If the 2D aluminum grating were coupled to an optimized nanoparticle SERS device fabricated from a DBCP NIL template, the coupled nanoparticle-grating device could exhibit an even higher enhancement and optical resonance performance.