Synchronization has been identified as a key aspect in social bonding. While synchronization could be maximized by increasing the predictability of an interaction, such predictability is in tension with individuals’ level of interest, which is tied to the interaction’s complexity and novelty. In this study, we tested the interplay between synchronization and interest. We asked 104 female dyads to play the Mirror Game, in which they had to move their hands as coordinately as possible, and then report how much they liked each other. Utilizing information theory and video processing tools, we found that a combination of movement synchronization and complexity explained liking almost two times better than movement synchronization alone. Moreover, we found that people initiated novel and challenging interactions, even though they paid a price—being less synchronized. Examining the interactions’ dynamics, we found that people who liked each other moved in a more synchronized, complex, and novel manner during most of the interaction. This suggests that in addition to synchronization, maintaining interest may be critical for positive social bonding. Thus, we propose a new framework in which balancing synchronization and interest, rather than merely maximizing synchronization, optimizes the interaction quality.