FullereneC60has stimulated intense interest for scientific, industrial, and medical community because of its unique structure and properties. In the present study we prepared fullerene-doped nanocomposite films based on PMMA, PVAc, and PMMA/PVAc blend. Observations made by transmission electron microscope (TEM) showed the uniform dispersion ofC60nanoparticles in the polymer matrices. Also, X-ray diffraction measurements indicated thatC60has a tendency to form crystallites in the polymer matrices. In addition, the concentration effect of fullereneC60was investigated using optical absorption and photoluminescence spectroscopy. The spectroscopic properties of such films recommended their application in photonics and solar energy conversion.