Golden inverse opals additionally decorated with 15.5 ± 1.5 nm gold nanoparticles are proposed as reusable substrates for surface-enhanced Raman spectroscopy (SERS). Gold nanoparticles are found to be uniformly distributed making an input of enhancement ability of spectral characteristics with the colloidal system by ten times. This technique is demonstrated to be efficient in spectral features tuning via a combination of different gold derivatives. Two lasers served for resonant, pre-resonance, and non-resonance signal analyses. Reusability of the Au-Au composite films is demonstrated for methylene blue as a stable dye deposited onto the SERS chips using a 632.8-nm resonant laser for exciting. The enhancement factor for methylene blue achieved 108 and for rohodamine 6G was of about 105. It was observed that rinsing of Au-Au nanocomposite SERS films with distilled water and heating up to 100 °C followed by dropping on a new portion of Au colloids onto the platform regenerates the substrates.