Graphene is a promising nanofiller for producing polymer nanocomposites with enhanced mechanical, electrical, thermal, electromechanical, and flame retardancy properties, leading to applications in aerospace, automotive, ballistics, medicine, electronics, and smart materials. Solvent-assisted top-down methods, including mechanical exfoliation of graphite, show great potential for scale-up and mass production of graphene dispersions for use in the fabrication of nanocomposites. However, these approaches can suffer from poor efficiency, which limits the concentrations of graphene/polymer dispersions that can be produced using in situ methods. As such, it is important to find new ways of making more effective use of these low concentrations of graphene nanofillers. Possible approaches include chemical modification of the graphene or finding synergies with other nanofillers to form hybrid nanocomposites. In this work, we demonstrate results that make use of each approach. Specifically, we demonstrate a low-cost and simple method for producing carbon nanotube dispersions and creating hybrid nanocomposites with substantial enhancements to mechanical properties. We also extend the scope of our previously reported semi-in situ exfoliation method by demonstrating its application in the production of a nanocomposite that incorporates chemically modified graphene. The superior mechanical properties exhibited by the nanocomposite are attributed to increased interaction strength between the polymer and nanofiller.