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Abstract Infancy is a sensitive period of development, during which experiences of parental care are particularly important for shaping the developing brain. In a longitudinal study ofN = 95 mothers and infants, we examined links between caregiving behavior (maternal sensitivity observed during a mother–infant free‐play) and infants’ neural response to emotion (happy, angry, and fearful faces) at 5 and 7 months of age. Neural activity was assessed using functional Near‐Infrared Spectroscopy (fNIRS) in the dorsolateral prefrontal cortex (dlPFC), a region involved in cognitive control and emotion regulation. Maternal sensitivity was positively correlated with infants’ neural responses tohappyfaces in the bilateral dlPFC and was associated with relative increases in such responses from 5 to 7 months. Multilevel analyses revealed caregiving‐related individual differences in infants’ neural responses to happy compared to fearful faces in the bilateral dlPFC, as well as other brain regions. We suggest that variability in dlPFC responses to emotion in the developing brain may be one correlate of early experiences of caregiving, with implications for social‐emotional functioning and self‐regulation. Research HighlightsInfancy is a sensitive period of brain development, during which experiences with caregivers are especially important.This study examined links between sensitive maternal care and infants’ neural responses to emotion at 5–7 months of age, using functional near‐infrared spectroscopy (fNIRS).Experiences of sensitive care were associated with infants’ neural responses to emotion—particularly happy faces—in the dorsolateral prefrontal cortex.