Over the past few decades, research studies have established that the mechanical properties of hydrogels can be largely impacted by the addition of nanoparticles. However, the exact mechanisms behind such enhancements are not yet fully understood. To further explore the role of nanoparticles on the enhanced mechanical properties of hydrogel nanocomposites, we used chemically crosslinked polyacrylamide hydrogels incorporating silica nanoparticles as the model system. Rheological measurements indicate that nanoparticle-mediated increases in hydrogel elastic modulus can exceed the maximum modulus that can be obtained through purely chemical crosslinking. Moreover, the data reveal that nanoparticle, monomer, and chemical crosslinker concentrations can all play an important role on the nanoparticle mediated-enhancements in mechanical properties. These results also demonstrate a strong role for pseudo crosslinking facilitated by polymer–particle interactions on the observed enhancements in elastic moduli. Taken together, our work delves into the role of nanoparticles on enhancing hydrogel properties, which is vital to the development of hydrogel nanocomposites with a wide range of specific mechanical properties.