Gold functionalized graphene oxide (GOAu) nanoparticles were reinforced in acrylonitrilebutadiene rubbers (NBR) via solution and melt mixing methods. The synthesized NBR-GOAu nanocomposites have shown significant improvements in their rate of curing, mechanical strength, thermal stability and electrical properties. The homogeneous dispersion of GOAu nanoparticles in NBR has been considered responsible for the enhanced thermal conductivity, thermal stability, and mechanical properties of NBR nanocomposites. In addition, the NBR-GOAu nanocomposites were able to show a decreasing trend in their dielectric constant (ε´) and electrical resistance on straining within a range of 10–70%. The decreasing trend in ε´ is attributed to the decrease in electrode and interfacial polarization on straining the nanocomposites. The decreasing trend in electrical resistance in the nanocomposites is likely due to the attachment of Au nanoparticles to the surface of GO sheets which act as electrical interconnects. The Au nanoparticles have been proposed to function as ball rollers in-between GO nanosheets to improve their sliding on each other and to improve contacts with neighboring GO nanosheets, especially on straining the nanocomposites. The NBR-GOAu nanocomposites have exhibited piezoelectric gauge factor (GFε´) of ~0.5, and piezo-resistive gauge factor (GFR) of ~0.9 which clearly indicated that GOAu reinforced NBR nanocomposites are potentially useful in fabrication of structural, high temperature responsive, and stretchable strain-sensitive sensors.