Pyridyl-terminated organic surface was created by self-assembling p-mercaptopyridine (p-MPy) onto sputtered gold substrates, on which well-defined gold nanoparticulate films were formed with a submonolayer coverage, as revealed by the tapping mode atomic farce microscopic (AFM) observations. Thus-prepared gold nanoparticulate films were shown to be active for surface enhanced Raman scattering (SERS), as evidenced by the strongly enhanced Raman scattering from the underlying SAMs. It might be the first report to demonstrate that colloidal gold nanoparticulate film can intrinsically enhance the Raman scattering of the molecules just below it.