This study reports the occurrence of 'tonal synchrony' as a new dimension of early mother-infant interaction synchrony. The findings are based on a tonal and temporal analysis of vocal interactions between 15 mothers and their 3-month-old infants during 5 minutes of free-play in a laboratory setting. In total, 558 vocal exchanges were identified and analysed, of which 84% reflected harmonic or pentatonic series. Another 10% of the exchanges contained absolute and/or relative pitch and/or interval imitations. The total durations of dyads being in tonal synchrony were normally distributed (M = 3.71, SD = 2.44). Vocalisations based on harmonic series appeared organised around the major triad, containing significantly more simple frequency ratios (octave, fifth and third) than complex ones (non-major triad tones). Tonal synchrony and its characteristics are discussed in relation to infant-directed speech, communicative musicality, pre-reflective communication and its impact on the quality of early mother-infant interaction and child's development.