The recent decade has seen a shift from artificial and environmentally deprived experiments in neuroscience to real-life studies on multiple brains in interaction, coordination and synchrony. In these new interpersonal synchrony experiments, there has been a growing trend to employ naturalistic social interactions to evaluate mechanisms underlying synchronous neuronal communication. Here, we emphasize the importance of integrating the assessment of neural synchrony with measurement of nonverbal behavioral synchrony as expressed in various social contexts: relaxed social interactions, planning a joint pleasurable activity, conflict discussion, invocation of trauma, or support giving and assess the integration of neural and behavioral synchrony across developmental stages and psychopathological conditions. We also showcase the advantages of magnetoencephalography neuroimaging as a promising tool for studying interactive neural synchrony and consider the challenge of ecological validity at the expense of experimental rigor. We review recent evidence of rhythmic information flow between brains in interaction and conclude with addressing state-of-the-art developments that may contribute to advance research on brain-to-brain coordination to the next level.