Although graphene-based materials have been used as fillers in polymer nanocomposites, a deleterious trade-off in mechanical strength and ductility is typically observed with increasing graphene loading, resulting in strong but brittle polymer nanocomposite materials. To provide outstanding compatibility with a standard high strength polymer, thermoplastic polyurethane (TPU), the use of a simple and mild sol-gel reaction to chemically attached silica nanoparticles to graphene oxide (GO) basal plane is reported. The silica modification imparts a highly porous GO surface structure, providing noncovalent attachment sites that improve physical entanglement between the GO and TPU. Furthermore, the silica modification enhances surface polarity, which imparts chemical affinity between the silica/GO nanocomposite and TPU. As a result, the prepared polymer nanocomposites exhibit significantly improved Young's modulus and tensile strength with only a small reduction of elongation at break over the neat polymer.