Background: Self-determination theory defines two important dimensions of teaching style: autonomy support and structure. Aims: The purpose of the present study was to investigate the synergistic relationship of perceived teacher autonomy support and the provision of structure in the prediction of self-regulated learning. Sample and method: Students (N = 526) completed questionnaires assessing perceived autonomy support, structure, and self-regulated learning. Results: First, autonomy support and structure were found to be positively correlated, suggesting that the support of student autonomy generally goes hand in hand with the provision of structure and order in the classroom. Second, moderated regression analyses indicated that structure but not autonomy support yielded a main effect on self-regulated learning, although this main effect was qualified by a structure by autonomy support interaction. Conclusion: The interaction suggests that structure was associated with more self-regulated learning under conditions of moderate and high autonomy support only. Therefore, when teachers want their students to evaluate themselves, to plan their study activities, and to think about themselves as learners, the teachers are encouraged to provide help, instructions, and expectations in an autonomy-supportive way.