Samples of chemically-vapor-deposited sub-micrometer-thick films of polysilicon were analyzed by transmission electron microscopy (TEM) in cross-section and by Raman spectroscopy with illumination at their surface. TEM and Raman spectroscopy both find varying amounts of polycrystalline and amorphous silicon in the wafers. Raman spectra obtained using blue, green and red excitation wavelengths to vary the Raman sampling depth are compared with TEM crosssections of these films. Some films have Raman spectra with a band near 497 cm−1, corresponding to numerous nanometer-scale faulted regions in the TEM micrographs.