High-density ordered core-sheath nanopillars of fullerene C60/C70 loading with colloidal Au nanoparticles were fabricated with a template method. The anodic aluminum oxide (AAO) template was first imbedded with the fullerene C60/C70 molecules and then followed by a pressure-difference approach for Au colloid. High-quality surface-enhanced Raman scattering (SERS) spectra of fullerene C60/C70 were obtained. The spectra show intense SERS signals with a fluorescence-free background, even with a 514 nm excitation at which the normal Raman of fullerene C60/C70 present poor signal-to-noise. The assembly of the fullerene C60/C70 on the inner walls of the AAO pores along the Au nanopillars lead to fluorescence quenching; meanwhile, the high-density and ordered arrays of Au nanopillars contribute to surface plasmon resonance for the SERS effect.