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The effect of brush thickness on the loading of gold nanoparticles (AuNPs) within stimuli-responsive poly-(N,N-(dimethylamino ethyl) methacrylate) (PDMAEMA) polyelectrolyte brushes is reported. Atom transfer radical polymerization (ATRP) was used to grow polymer brushes via a “grafting from” approach. The brush thickness was tuned by varying the polymerization time. Using a new type of sealed reactor, thick brushes were synthesized. A systematic study was performed by varying a single parameter (brush thickness), while keeping all other parameters constant. AuNPs of 13 nm in diameter were attached by incubation. X-ray reflectivity, electron scanning microscopy and ellipsometry were used to study the particle loading, particle distribution and interpenetration of the particles within the brush matrix. A model for the structure of the brush/particle hybrids was derived. The particle number densities of attached AuNPs depend on the brush thickness, as do the optical properties of the hybrids. An increasing particle number density was found for increasing brush thickness, due to an increased surface roughness.