Surface roughness of metal nanoparticles (NPs) is well-known to play an important role in the quantitative analysis and performance of their surface-enhanced Raman scattering (SERS), but its analogous role in catalysis is not given the due credit yet. In the present work, we systematically investigated this by utilizing two significantly relevant gold (Au) nanostructures, hollow and star-shaped, in a comprehensive manner. For catalysis, the universal model reaction, the reduction of p-nitroaniline to phenylenediamine using NaBH4, was engaged and SERS measurements were performed by employing methylene blue as the standard analyte molecule. At the outset, the predominantly fascinating role of the nanoparticle surface area in conjunction with surface roughness in catalysis was carefully evaluated for our robustly synthesized Au hollow nanoparticles (NPs), possessing an inherent thin inner core layer of Ag, and star-shaped Au NPs along with two different-sized solid spherical Au NPs. As expected, improved per...