Silver-doped silicon thin films were deposited on glass substrate in a co-sputtering procedure. Silver nanoparticles were segregatedly distributed. The nonlinear properties were extracted by z-scan measurements at low laser input power. For about 50% silver density, the nonlinear absorption and refraction coefficients peaked, respectively, at −8.086 × 10 −2 m/W and 1.47 × 10 −9 m 2 /W, which, with respect to the input intensity, are several orders higher than reported data. The sudden surge of nonlinear responses was explained satisfactorily based on a self-consistent microscopic model calculation for silver clusters. Resonances exist and depend apparently on the laser-modified local cluster concentration.