The surface-enhanced Raman scattering (SERS) properties of 4-aminothiophenol (PATP) adsorbed on self-assembled cobalt nanoparticle chains have been investigated. Based on the density functional theory (DFT), the experimental results were in good agreement with the calculated values of the characteristic bands both for normal Raman and SERS spectra. The enhancement factor (EF) of 10(4)-10(5) indicated that high quality of surface Raman signals could be obtained, which was consistent with discrete-dipole approximation (DDA) calculation results. The SERS substrate may be helpful for extending SERS to transition metals and offering some promising applications of SERS in the future.