Polymer brushes are classifically defined and are to date employed as assembliles of macromolecules tethered at one end to a surface. The concept of preparing surface-grated gels by crosslinking such brushes is attractive since it gives rise to new opportunites related to the constraints present in this type of structure. Aiming at the development of nanostructured films possessing precisely adjustable chemical, mechanical, and optical properties, the present article describes the preparation of novel grated layers based on gel-brush/metal nanoparticle hybrids. These films were synthesized by surface-initiated atom transfer radical polymerization of hydroxyethyl methacrylate with a small percentage of a crosslinker. The swelling morphological, and mechanical properties of the gel-brushes are shown to be highly dependent on the relative amount of crosslinker used. The gel-brushes are subsequently used as matrixes for the controlled synthesis of silver nanoparticles with overall characterisitics that are specifically tunable as a function of the macromolecular structure of the brush template.