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Process mining analysis was adopted to gain deep insights into the relations between teachers’ self-regulated learning (SRL) and their development of technological pedagogical content knowledge (TPACK) in a computer-supported learning environment. Seventy participants were classified based on their TPACK achievements measured by self-reported TPACK competencies and evaluations of lesson plans. Raw computer logs were used to make an inference to seven fine-grained SRL events. Results indicated that teachers with higher TPACK achievements were more regulated during designing plans. Implications are discussed with respect to improving teachers’ SRL during knowledge acquisition in the context of a computer-supported learning environment.