Interpersonal synchrony serves as a subtle, yet powerful bonding mechanism in social interactions. Problematically, the term ‘synchrony’ has been used to label a variety of distinct aspects of interpersonal coordination, such as postural similarities or movement activity entrainment. Accordingly, different algorithms have been suggested to quantify interpersonal synchrony. Yet, it remains unknown whether the different measures of synchrony represent correlated features of the same perceivable core phenomenon. The current study addresses this by comparing the suitability of a set of algorithms with respect to their association with observers’ judgments of dyadic synchrony and leader-followership. One-hundred fifteen observers viewed computer animations of characters portraying the movements of real dyads who performed a repetitive motor task with instruction to move in unison. Animations were based on full-body motion capture data synchronously collected for both partners during the joint exercise. Results showed most synchrony measures significantly correlated with (a) perceived synchrony and (b) the perceived level of balance of leading/following by each dyad member. Phase synchrony and Pearson correlations were associated most strongly with the observer ratings. This might be typical for intentional, structured forms synchrony such as ritualized group activities. It remains open if these findings also apply to spontaneous forms of synchrony as, for instance, occurring in free-running conversations.