The formation of nanocomposites by embedding inorganic nanoparticles (NPs) in polymer brushes has been studied extensively for the development of functional surfaces. Polymer brushes are particularly useful matrices for the preparation of nanocomposites, because the macromolecular matrix acts as a reaction chamber for nanoparticle synthesis, as a scaffold for immobilization, and as a capping agent for preventing nanoparticle aggregation. Moreover, synergies between the polymer chains and the inorganic NPs will grant the composite new properties. The stimuli-responsive polymers/NPs endow the composites with excellent properties for many applications, such as in sensors, detectors, and electronic/optical devices. We tackle in this review the use of a subset of polymer brushes (e.g., polyelectrolytes and polyampholytes) for the embedment of inorganic NPs to make composite surfaces/NPs with specific functions.