On-line comprehension of natural speech requires segmenting the acoustic stream into discrete linguistic elements. This process is argued to rely on theta-gamma oscillation coupling, which can parse syllables and encode them in decipherable neural activity. Speech comprehension also strongly depends on contextual cues that help predicting speech structure and content. To explore the effects of theta-gamma coupling on bottom-up/top-down dynamics during on-line syllable identification, we designed a computational model (Precoss—predictive coding and oscillations for speech) that can recognise syllable sequences in continuous speech. The model uses predictions from internal spectro-temporal representations of syllables and theta oscillations to signal syllable onsets and duration. Syllable recognition is best when theta-gamma coupling is used to temporally align spectro-temporal predictions with the acoustic input. This neurocomputational modelling work demonstrates that the notions of predictive coding and neural oscillations can be brought together to account for on-line dynamic sensory processing.