A synthetic route of sol-gel towards the fabrication of bimetallic gold plus nickel nanoparticles (NPs) in sodium borosilicate glass is presented, with the need of controlled atmosphere heat treatments.Characterization of the as-obtained glasses by X-ray powder diffraction (XRD), Transmission electron microscopy (TEM) and X-ray photoelectron spectroscopy (XPS) indicate that when exposed to variable atmosphere of oxygen (O2) and oxygen (O2)-hydrogen (H2), randomly distributed Au/NiO NPs and Au/Ni NPs are produced in the glass host, respectively.Subsequently, the Z-scan technique is conducted to examine the nonlinear optical response of the resulting glasses at 800 nm with 190 fs pulses.Interestingly, the two glasses behave better optical nonlinearities comparable to that of the glass incorporated into only Au NPs.For sodium borosilicate glass dispersed with Au/NiO NPs, the enhancement of the third-order nonlinear response depends mainly on a contribution of stronger nonlinear refraction response.Yet, the dominant contribution to improve optical nonlinearities of sodium borosilicate glass dispersed with Au/Ni NPs is more intense nonlinear absorption effect.This work would suggest a promising way to fabricate more pronounced nonlinear materials and offer strong potential for future photonics.