In this study, gold nanoparticles (GNPs) were successfully fabricatedviaa polymer-templating method and applied for surface-enhanced Raman scattering (SERS) enhancement. The block copolymer, poly(ethylene glycol)-block-poly(styrene-alt-maleic anhydride) (PEG-b-PSM) modified with thiol groups, was used to prepare GNPs. The results indicated that the polymer facilitated GNPs to form an assembly without aggregation; thus, the distance between adjacent GNPs could be ideal for SERS application. Furthermore, when deposited onto indium tin oxide (ITO) thin film, GNPs preparedviathe polymer-templating method showed more ordered behavior than GNPs prepared by using a conventional method, that is, citrate reduction.