The unique properties of a polymer photonic crystal are examined with respect to applications as a medium for high-density three-dimensional optical data storage media. The nanocomposite material was produced from core-shell latex particles, in which the latex cores contained dye-labeled polymer. Nonfluorescent latex shells were attached to the core particles. Upon annealing, the close-packed core-shell particles formed a nanostructured material with the fluorescent particles periodically embedded into the optically inert matrix in a hexagonal close-packed structure. A two-photon laser scanning microscope was used to write bits of information into the material by photobleaching the optically sensitive particles and, under much lower fluence, read out the resulting image. Relative to conventional homogeneous storage media, the nanostructured periodic material is shown to increase the effective optical storage density by at least a factor of 2 by spatially localizing the optically active region and imposing an optically inactive barrier to cross-talk between bits. This polymer photonic crystal has the potential to dramatically improve performance further through the improved capabilities to optimize the photochemical processes and more fully exploiting the periodic nature of the information domains in the image processing.