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This paper examines the role of self-regulation in teachers’ development of technological pedagogical content knowledge (TPACK). In particular, we explore the relationship between teachers’ self-regulated learning and teaching. Educational data mining was applied to mine the self-reported data as a means to identify distinct teacher profiles of teachers’ self-regulation and TPACK respectively. Chi-square tests revealed that teachers who are more capable to regulate their own learning reported greater proficiency in using technologies in the classroom. We discuss the implications for designing adaptive instructional support in the context of computer-based learning environments.