Keeping in view the fascinating properties of noble materials in the nanoscale, we synthesized nanocomposite materials from metals of Au and Ag in the form of core/shell structure by a simple, eco-friendly, inexpensive, smart, and fast method. This method is pulsed laser ablation of Ag plate immersed in chloroauric acid solution using Nd:YAG solid state laser (1064nm, 7ns, 10Hz). The physicochemical investigations were presented by different techniques to investigate its structural characterization, morphological and optical characterization including linear and nonlinear properties. These techniques confirmed that produced sample has a crystalline structure from Au an Ag structure, and its morphology has a core/shell structure with Au in shell and Ag in core. The nonlinear optical characterization of the prepared sample was investigated by Z-scan technique using the second harmonic of the same laser source. The prepared sample of Au@Ag core/shell showed a tuning of nonlinearity characteristic property between that of the nanoparticles from Au or Ag. So, this material could be represented a recommended nonlinear material to be a promising candidate for optical limiting applications