Detection of important biological molecules using surface-enhanced Raman scattering (SERS) has become widely used because of the highly sensitive and label free approach offered by SERS as well as the low cytotoxic response from some SERS substrates. Gold nanoparticles are commonly used in SERS studies; however, the inherent instability of these metal nanostructures in solution adversely influences the reproducibility and quantitative nature of these measurements. Furthermore, the metal surface often denatures biomolecules upon their direct interaction. To combat this incompatibility and improve optical stability, gold nanoparticles have been encapsulated in silica shells. These Au@SiO2 nanostructures have been used extensively in cellular studies, but their SERS capabilities are generally limited to uses that include silica-entrapped SERS reporter molecules rather than direct SERS detection. This work focuses on combating these limitations via the fabrication of Au@SiO2 nanoparticles with porous silica membranes for the direct detection of target molecules in solution. Gold nanoparticles have been designed and coated with a variety of silica morphologies and subsequently interrogated using extinction spectroscopy and SERS. It will be revealed that these gold nanoparticles entrapped in silica membranes serve as optically stable substrates for the quantitative and direct detection of target molecules. These advances in nanomaterial fabrication are envisioned to impact both fundamental and applied studies in a variety of research areas including catalysis, separations, and spectroscopy.