Polymer nanocomposites (PNCs), prepared by incorporating nanoparticles within a polymer host, generally exhibit properties that differ significantly from those of the host, even with small amounts of nanoparticles. A significant challenge is how to tailor the properties of these materials for applications (structural and biomedical to optoelectronic), because PNCs derive their properties from a collective and complex range of entropic and enthalpic interactions. Here, we show that PNCs, prepared from athermal mixtures of polymer-chain-grafted gold nanoparticles and unentangled polymer chains, may exhibit increases or decreases in their relaxation dynamics, and viscosity, by over an order of magnitude through control of nanoparticle concentration, nanoparticle size, grafting density and grafting chain degree of polymerization. In addition, we show how the glass transition may also be tailored by up to 10 degrees with the addition of less than 1.0 wt% nanoparticles to the polymer host.