We have studied the applicability of Fourier transform (FT)-Raman spectroscopy to the determination of isotacticity in polypropylene. We have compared FT-Raman and Fourier transform infra-red (FTi.r.) spectroscopy as isotacticity determination methods and used C-13 nuclear magnetic resonance (n.m.r.) spectroscopy as a reference method. Calibration curves relating Raman scattering and i.r. absorption ratios to the C-13 n.m.r. results are presented. We found that the repeatability for both FT-Raman and FTi.r. measurements is comparable to that of C-13 n.m.r. analysis and that there is a good correlation between C-13 n.m.r. and FT-Raman/FT-i.r. results. The reliabilities of the three methods are statistically evaluated and compared.