Graphene Oxide (GO) and aminosilane (AS) modified GO (GOAS) have been studied as possible compatibilizers for immiscible polyblends based on Polypropylene (PP) / Polyamide (PA). The localization of the nanoparticles (NPs) within the polyblend's phases is of utmost importance for optimal compatibility and enhanced properties. For control of the localization of the NPs at the interface of a PA/PP system the thermodynamics of the constituents and mixing dynamics have to be tailored. Accordingly, a variety of oxidation levels (10 - 40%) of GOs were prepared using Hummer's method and were further modified by AS in aqueous media. Experimental results indicated that the GO goes through thermal reduction (above 200oC) during blending and reduced GO is obtained. The AS modified GO moderated the reduction reaction resulting in stabilizing the GO. The thermodynamic wetting coefficient of the PP/PA/rGOAS system was shown to drive the rGOAS to the blend's interface during time controlled blending. The localization of the rGOAS at the interface resulted in significant enhancement of mechanical properties using only 2-3 wt. % of rGOAS and displayed 75% enhancement in strength and 45% enhancement in modulus compared to neat PP/PA. At this concentration range of the rGOAS a rheological percolated network was obtained. Scanning electron microscopy of the fracture surfaces supported the mechanical properties enhancement displaying a homogeneous structure with the nanoparticles mostly situated at the PA/PP interface.