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The present investigation is aimed to develop hybrid nanocomposites of polyetherimide (PEI)/silicone rubber (85:15 wt:wt) incorporated with fixed loading (3 wt%) of halloysite nanotubes (HNTs) and 0.0, 0.1, 0.3, and 0.5 wt% loadings of reduced graphene oxide (RGO) by melt mixing process using a twin-screw extruder. In comparison with RGO, it is observed that the HNTs disperse sparingly in PEI/silicone rubber mixtures in spite of having similar Physico-chemical structures. SEM studies reveal that the addition of RGO increases the dispersion of HNTs in PEI/silicone rubber to a greater extent, which results in an improvement in tensile strength from 41 to 59 MPa and tensile modulus from 658 to 715 MPa on the addition of 0.3 wt% of graphene. This synergistic effect of both the nanofillers is also reflected by significant improvements in flexural modulus (from 3217 to 4156 MPa), impact strength (56 to 78 J/m), Rockwell hardness (89 to 104), and thermal properties of nanocomposite; the highest storage modulus (7290 MPa) was observed for 0.3 wt% and lowest (5390 MPa) for 0.0 wt% loading of graphene at 50 °C temperature. It is due to the rigidity in polymer chains movement because of dispersion of RGO that improves the interfacial interaction, as well as thermal vibrations of the C–C bond, which are restricted of the polymer matrix. [ABSTRACT FROM AUTHOR]