Infant-adult synchrony has been reported through observational and experimental studies. Nevertheless, synchrony is addressed differently in both cases. While observational studies measure synchrony in spontaneous infant-adult interactions, experimental studies manipulate it, inducing nonspontaneous synchronous and asynchronous interactions. A still unsolved question is to what extent differ spontaneous synchrony from the nonspontaneous one, experimentally elicited. To address this question, we conducted a study to compare synchrony in both interactional contexts. Forty-three 14-month-old infants were randomly assigned to one of two independent groups: (1) the spontaneous interaction context, consisting of a storytime session; and (2) the nonspontaneous interaction context, where an assistant bounced the infant in synchrony with a stranger. We employed an optical motion capture system to accurately track the time and form of synchrony in both contexts. Our findings indicate that synchrony arising in spontaneous exchanges has different traits than synchrony produced in a nonspontaneous interplay. The evidence presented here offers new insights for rethinking the study of infant-adult synchrony and its consequences on child development.