The copolymerization of styrene and acrylonitrile in bulk at 60 °C has been investigated by measurement of the copolymer/comonomer composition relationship and of the monomer sequence distributions using 13C NMR. Alternative models for the mechanism of the copolymerization have been evaluated in the most general forms, with allowance for nonzero conversions, by deriving reactivity ratios from composition data and then comparing predicted and experimental sequence distributions. The system shows significant deviations from the terminal model. Compositions cannot differentiate between penultimate and complex participation models, both of which give significant improvement over the terminal model. The measured sequence distributions are quite close to the predictions of the penultimate model but substantially different from those of the complex participation model, showing clearly that the penultimate model is the most appropriate of the models considered. We have obtained rss = 0.22g, rM = 0.03g, r^= 0.634, and rSA = 0.09v No significant improvement was observed with the antepenultimate model.