When infants and toddlers are confronted with sequences of sounds, they are required to segment the sounds into meaningful units to achieve sufficient understanding. Rhythm has been regarded as a crucial cue for segmentation of speech sounds. Although previous intermodal methods indicated that infants and toddlers could detect differences in speech sounds based on stress-timed and syllable-timed units, these methods could not clearly indicate how infants and toddlers perform sound segmentation. Thus, the present study examined whether Japanese infants and toddlers could segment word speech sounds comprising basic morae (i.e., rhythm units similar to syllables), on the basis of concurrent basic mora units within syllable units, using the new intermodal matching procedure. The results indicated that, regardless of their ages and linguistic abilities, Japanese infants and toddlers aged 6–25 months tended to segment Japanese words comprising basic morae sounds on the basis of concurrent basic mora units within syllable units. This implies that infants' and toddlers' use of syllable units for segmentation of speech sounds at an early age could be evident among many infants and toddlers learning various languages. Although this finding should be interpreted carefully, the present study demonstrated the utility of the new intermodal matching procedure for examining segmentation of speech sounds and word sounds by infants and toddlers, on the basis of specific rhythm units.