The grafting of polymeric chains to inorganic (as well as organic) particle interfaces has become an indispensable tool to engineer the physicochemical and/ or biochemical properties of material interfaces. For example, polymer grafting is ubiquitously being used to compatibilize particles to polymer matrices to augment the properties of polymers in applications such as biomedical devices, lightweight aircraft wings, energy generation and storage, and for separation and environmental remediation to name a few. The recent emergence of surface-initiated controlled radical polymerization has further expanded the scope of polymer-grafted particulate materials, as the precise control of the structure of the polymer grafts offers new opportunities to tailor the properties of polymer-grafted particle systems. This chapter summarizes recent developments in synthesis of polymer-tethered nanoparticle interfaces that have afforded this fine control in the structure and properties of the resultant composite. Particular emphasis is given to the concept of "one-component hybrid materials"-that is the ability to synthesize multifunctional nanocomposite materials by the self-assembly of polymer-tethered particle systems. The role of polymer-graft modification on the interaction, dynamics, and assembly of particle brush materials is discussed to provide the context to showcase studies that have demonstrated the opportunity to harness the precision-engineered polymergrafted particle systems for the fabrication of innovative nanocomposite material technologies.