This paper reports an effective method to enhance the surface plasmon resonance (SPR) on Ag films by using a thin Ni seed layer assisted deposition. Ag films with a thickness of about 50 nm were deposited by electron beam evaporation above an ultrathin Ni seed layer of approximately 2 nm on both silicon and quartz substrates. The root-mean-square (rms) surface roughness and the correlation length have been reduced from >4 nm and 28 nm for a pure Ag film to approximately 1.3 and 19 nm for Ag/Ni films, respectively. Both experimental and simulation results show that the Ag/Ni films exhibit an enhanced SPR over the pure Ag film with a narrower full width at half-maximum. Ag films with a Ge seed layer have also been prepared under the same conditions. The surface roughness can be reduced to less than 0.7 nm, but narrowing of the SPR curve is not observed due to increased absorptive damping in the Ge seed layer. Our results show that Ni acts as a roughness-diminishing growth layer for the Ag film while at the same time maintaining and enhancing the plasmonic properties of the combined structures. This points toward its use for low-loss plasmonic devices and optical metamaterials applications.