This study investigated the interplay of temporal changes in self-regulated learning processes (i.e., behavioral, cognitive, motivational and emotional) and their relationship with academic achievement in computer-supported collaborative learning. The study employed electrodermal activity and self-report data to capture the dynamicity of self-regulated learning processes during 15 sessions of collaborative learning activities. Our findings revealed that the changes in motivational regulation was related to academic achievement. However, academic achievement was not related to behavioral regulation, cognitive regulation or emotional regulation. Physiological synchrony among the collaborating students was found to be related only to cognitive regulation. The results also showed that the concordance of self-report data among the collaborating students was related to higher physiological synchrony among them in the behavioral, cognitive, and motivational dimensions of self-regulated learning. The findings reflect the complexity of the relationships between self-regulated learning constructs and demonstrates the potential value of physiological measures in self-regulated learning research.