Surfaces serve as the communication link between the adsorbate and the substrate. Hence, a thorough understanding of the surface chemistries directly interfacing with biological molecules and other adsorbates would provide insight into the fabrication approach as well as the adsorption characteristics of biomolecules adsorbed on the surface. This paper presents a surface-enhanced Raman spectroscopy (SERS) method for high-sensitivity detection and reading of protein microarrays based on gold nanoparticle labels. The reagent employed was 30 nm gold nanoparticles modified with a bifunctional Raman reporter molecule, 5,5'-dithiobis(succinimidyl-2-nitrobenzoate) (DSNB), to integrate anti-bovine IgG for an antigen response in the immunoassay and generate an intense SERS signal. The signal from the DSNB reporter molecule, particularly the strong symmetric nitro stretch was used for the detection of antigen-antibody interactions. Issues related to the sensitivity and selectivity of the assay were also addressed. This work provides useful insights into SERS-based immunoassays and serves as the basis for an eventful adventure into interfacial biomolecular interactions.