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We hypothesize that effective collaboration is facilitated when individuals and environmental components form a synergy where they work together and regulate one another to produce stable patterns of behavior, or regularity, as well as adaptively reorganize to form new behaviors, or irregularity. We tested this hypothesis in a study with 32 triads who collaboratively solved a challenging visual computer programming task for 20 min following an introductory warm‐up phase. Multidimensional recurrence quantification analysis was used to examine fine‐grained (i.e., every 10 s) collective patterns of regularity across team members' speech rate, body movement, and team interaction with the shared user interface. We found that teams exhibited significant patterns of regularity as compared to shuffled baselines, but there were no systematic trends in regularity across time. We also found that periods of regularity were associated with a reduction in overall behavior. Notably, the production of irregular behavior predicted expert‐coded metrics of collaborative activity, such as teams' ability to construct shared knowledge and effectively negotiate and coordinate execution of solutions, net of overall behavioral production and behavioral self‐similarity. Our findings support the theory that groups can interact to form interpersonal synergies and indicate that information about system‐level dynamics is a viable way to understand and predict effective collaborative processes. [ABSTRACT FROM AUTHOR]