Fullerene C60 has 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 of C60 nanoparticles in the polymer matrices. Also, X-ray diffraction measurements indicated that C60 has a tendency to form crystallites in the polymer matrices. In addition, the concentration effect of fullerene C60 was investigated using optical absorption and photoluminescence spectroscopy. The spectroscopic properties of such films recommended their application in photonics and solar energy conversion.