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We describe the fabrication of optimized plasmonic substrates in the form of immobilized nanorod assemblies (INRA) for surface-enhanced Raman spectroscopy (SERS). Induded are high-resolution scanning electron micrograph (SEM) images of the surface structures, along with a mechanistic description of their growth. It is shown that, by varying the size of support microspheres, the surface plasmon resonance is tuned between 330 and 1840 nm. Notably, there are predicted optimal microsphere sizes for each of the commonly used SERS laser wavelengths of 532, 633, 785, and 1064 nm. [ABSTRACT FROM AUTHOR]