We report the first evidence of Raman scattering from surface phonons of a pristine metal surface. Our study reveals a Raman-active surface vibrational resonance on Cu(110) with a surprisingly large scattering efficiency. With the incident photon energy close to the energy of the Cu(110) surface state electronic transition, the Raman scattering from the surface optical resonance can be significantly enhanced, while any contribution from bulk phonons is absent.