Addition of nanoparticles into polymers can produce materials with new and enhanced properties. It has been widely shown that the nanofiller–matrix polymer interactions and the dispersion state of nanoparticles play an important role on the final properties of the nanocomposite system. Recently, we observed a unique thermal stiffening behavior in a poly(ethylene oxide), PEO, based nanocomposite, which contained poly(methyl methacrylate), PMMA, adsorbed silica nanoparticles. The thermal stiffening behavior was observed for samples that were carefully prepared via solution mixing to ensure that the PMMA would be adsorbed to nanosilica prior to being mixed with PEO. Although the thermal stiffening behavior was found to be repeatable under cyclic thermal loading, it is not clear if the PEO/PMMA/nanosilica layered structure would survive under continuous processing conditions. Therefore, in the current study, we processed two different nanocomposites at varying shear rates via melt extrusion. The structure of processed samples was characterized with small angle X-ray scattering and scanning electron microscopy, and their viscoelastic properties were investigated via rotational rheometry. Results indicate that state of dispersion of silica nanoparticles, and adsorbed and matrix polymer chemistries strongly influenced samples’ response to extrusion. This material is based upon work supported by the National Science Foundation under Grant No. CMMI-1825254.