The past couple of decades produced a surge of interest in interaction synchrony. Moving from the study of behavioral coordination to investigating the coordination of psychophysiological and brain activity, relevant research has tackled a broad range of interactional settings with a multitude of measurement and analysis tools. This method diversity produced a host of interesting results converging on the fact that individuals engaged in social exchange tend to temporally align external as well as internal processes. Moreover, there appears to be a reciprocal relationship between the individuals’ affective bond and the extent of synchronization, which together benefit interaction outcomes. Notably, however, the current breadth of study approaches creates challenges for the field, including how to compare findings and how to develop a theoretical framework that unites and directs ongoing research efforts. More concerted efforts are called for to achieve the conceptual and methodological clarity needed to answer core questions and enabling a balanced pursuit of both synchronous and asynchronous processes.