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Teaching is an inherently interactive phenomenon and a social-emotional cognitive skill. Using a dynamic systems and social-emotional cognitive lens, this study borrows methods from interaction studies to identify periods of psychophysiologic synchrony between the teachers and students to determine if these correlated with their relational experiences. The results demonstrated significant increases of psychophysiologic synchrony in the teacher–student dyads that were engaged in a supported teaching task. This elevated synchrony was correlated with multiple domains of two established measures of individual social-emotional cognition. These data indicated that the ability to create synchrony during supported interactions was connected to the teacher’s distinct social-emotional cognitive capacity. These results also support the potential neurobiologic and psychophysiologic bases of teachers’ social-emotional cognitive processing.