Anodic aluminum oxide (AAO) templates were employed to filtrate and assemble Au nanoparticles by the pressure difference method. It was found that the colloidal Au nanoparticles can be uniformly arranged as nanonet assembly on the AAO surface. The net-assembled Au nanoparticles are clean and closely packed with nanochains. Taking fullerene C60/C70 as probe molecules, high-quality surface-enhanced Raman scattering (SERS) spectra were observed. The net-assembled Au nanoparticles even synchronously support the observation of surface-enhanced infrared absorption (SEIRA) spectra of the fullerene C60/C70. These results indicate that the AAO template filtrated with net-assembled Au nanoparticles is a highly active substrate for surface-enhanced spectroscopy.