As social beings, we are adept at coordinating our body movements and gaze with others. Often, when coordinating with another person, we orient ourselves to face them, as mutual gaze provides valuable cues pertaining to attention and intentions. Moreover, movement synchrony and mutual gaze are associated with prosocial outcomes, yet the perceptual consequences of these forms of coordination remain poorly understood. Across two experiments, we assessed how movement synchrony and gaze direction influence observers’ perceptions of dyads. Observers’ behavioural responses indicated that dyads are perceived as more socially connected and are more enjoyable to watch when moving synchronously and facing each other. Neuroimaging results showed modulation of the Action Observation and Theory of Mind networks by movement synchrony and mutual gaze, with more robust brain activity when evaluating togetherness (i.e., active and intentional collaboration) than aesthetic value (i.e., enjoyment). A fuller understanding of the consequences of movement synchrony and mutual gaze from the observer’s viewpoint holds important implications for social perception, in terms of how observers intuit social relationships within dyads, and the aesthetic value derived from watching individuals moving in these ways.