Surface-enhanced Raman spectra of pyridine on copper and gold electrodes in the near-infrared were obtained with a Fourier transform Raman spectrometer. Surface-enhanced Raman spectra were observed for pyridine adsorbed on copper and gold electrodes while a Nd:YAG laser (1.064/μm) was used for excitation. Good-quality spectra were recorded for 0.08 mM pyridine on a copper electrode with a single oxidation-reduction cycle, whereas for a gold electrode, several ORCs were necessary. A very intense low-energy Raman band was observed on both metals at positive potentials, which may be due to a metal-oxide vibrational mode.