Silver nanocomposites are synthesized by the gelation of a homogeneous dispersion of presynthesized nanoparticles in a hydrogel-forming monomer solution containing acrylamide and N,N-methylenebisacrylamide. The molecular interactions present in the nanocomposites are characterized by UV-Vis and FT-IR spectroscopic methods. Quantitative results on the thermophysical, mechanical and deswelling properties of the nanocomposites are presented. Differential scanning calorimetric results show unexpected thermal properties of water present in the nanocomposites, indicating the potential of these nanocomposites for cold storage applications. The nanocomposites are observed to become significantly more ductile in nature with an increasing concentration of nanoparticles. The deswelling kinetics of the nanocomposites indicate that they deswell relatively faster than the base material. Upon exposure to solar radiation, the nanocomposites provide a temperature increase of 3.6 ± 1.0 °C over the base material, suggesting that the silver nanoparticles can act as a nanoboiler.