Bare gold nanoparticles were embedded into an iron-polyoxovanadate matrix and used to enhance both the infrared and Raman signatures of a model analyte. A detailed characterization of the matrix-embedded nanoparticles revealed that they retained a plasmon resonance at 564 nm. The enhancement of vibrational signatures of the model analyte crystal violet using bare and embedded gold nanoparticles was compared for both surface enhanced infrared (SEIRA) spectroscopy and surface enhanced Raman spectroscopy (SERS) yielding enhancement factors of 2.2 for SEIRA and 77 for SERS. In contrast, the bare gold nanoparticles revealed significantly lower enhancements (1.6 for SEIRA; 20 for SERS). Hence, it was shown that embedding nanoparticles within an inorganic polyoxometalate-based matrix is an innovative strategy to amplify their signal enhancement properties in vibrational spectroscopies.