Changes in the Raman spectra of quenched poly(tetrafluoroethylene) have been correlated with the crystallinity by differential scanning calorimetry, i.r. spectroscopy, density, and wide-angle X-ray scattering. An increasing tailing of the band at Delta v=1381 cm(-1) (CF2 symmetric stretching fundamental) has been identified as the most marked effect of decreased crystallinity. A method for quantifying the band tailing has been devised. It was found that the band tailing so quantified can serve as a measure for the crystallinity.