Notably Au@CloseLarge has a higher enhancement in SERS signal compared to the other SPs, which is in line with expectation based on the EELS data. On the other hand, the weight-based deposition may have an influence on the number of nanoparticles available for Au@DistantSmall. Still, despite being closely spaced, Au@CloseSmall SPs show a lower SERS enhancement compared to Au@CloseLarge, indicating that the plasmonic coupling in larger SPs with closely spaced plasmonic nanoparticles leads to greater near-field enhancement.