Nanocomposite thin films consisting of Au nanoparticles embedded in yttria-stabilized zirconia (YSZ) were synthesized at room temperature by radio frequency magnetron co-sputtering from YSZ and Au targets and subsequently annealed in an argon atmosphere. Au microstructure and particle size were characterized as a function of annealing temperature from 600 to 1000 °C by x-ray diffraction, transmission electron microscopy, scanning electron microscopy, and Rutherford backscattering spectroscopy. Spectroscopic ellipsometry was also used to determine the optical constants of the resulting films. In particular, the refractive index of the nanocomposites was found to undergo an anomalous dispersion in the spectral region where the extinction coefficient achieves its maximum. Additionally, the incorporation of Au in the YSZ matrix was found to increase the refractive index in comparison to that of YSZ. At annealing temperatures higher than 800 °C, a good agreement was found between experimental findings and theoretical models using bulk dielectric functions for Au, as modified to account for a reduced mean free path for scattering than that for free electrons. However, for annealing temperatures below 800 °C, an additional offset was required for the optical constants of Au to obtain good agreement between theory and experiment. This behavior was attributed to a relatively high atomic Au concentration in the YSZ matrix.