The phase behavior of a molecular brush-C-18 grafted to the surface of both a silicon wafer and SiO2 nanoparticles was investigated as a function of temperature using neutron reflectometry (NR) and small-angle neutron scattering (SANS), respectively. The experiments demonstrate a phase change in the brush layer characterized by a straightening of the molecular configuration, increase in shell thickness, and increase in solvent concentration with decreasing temperature that corresponds to gelation in the nanoparticle dispersion.