The utility and efficacy of thermoresponsive poly(N-isopropylacrylamide) (PNIPAAm) hydrogels as smart materials is limited by their physical properties. In this study, we sought to design PNIPAAm nanocomposite hydrogels which displayed enhanced mechanical properties as well as deswelling–reswelling kinetics but without reducing equilibrium swelling or altering the convenient volume phase transition temperature (VPTT) of PNIPAAm. PNIPAAm hydrogels were formed as double networks (DN) comprised of a tightly crosslinked 1st network and a loosely crosslinked 2nd network. In addition, polysiloxane nanoparticles of two different average diameters (50 nm and 200 nm) were incorporated during formation of the 1st or 2nd network. The influence of the hydrogel composition on VPTT, morphology, equilibrium swelling, deswelling–reswelling kinetics and mechanical properties was evaluated. We observed that DN hydrogels formed with 200 nm polysiloxane nanoparticles introduced during formation of the 1st network achieved the best combination of the desired properties.