Gold nanoparticles with enhanced efficiency as substrates for surface-enhanced Raman and infraredspectroscopies have been grown by pulsed laser deposition on glass and CaF2 substrates. Transmission electronmicroscopy analysis has evidenced the presence of nanoparticles with characteristic sizes of several nanometersin diameter. The capabilities of the produced nanoparticles as enhancer substrates have been investigatedusing the dithiocarbamate fungicide thiram as a test molecule. The enhancement factors and features of SERSand SEIRA spectra are compared to those observed from large Au nanoparticles produced by evaporation athigh temperatures. Slight changes in favor of the new substrates are discussed.