Early life experiences influence brain function and structure throughout life. Maternal signals constitute a major source of early life experiences, and their quantity and qualities during sensitive developmental periods exert enduring effects on infant, child and adult emotional and social behaviors in humans, primates and rodents. Existing studies probing the salient qualities of maternal signals to the infant have centered primarily on measures of their valence. Here we report that in addition to these established qualitative dimensions, patterns of maternal signals contribute greatly to infants and children’s self-control, a potent predictor of mental health outcomes. In two large, independent and disparate prospective cohorts in Turku, Finland, and Irvine, CA, USA, unpredictable sequences of maternal care portended worse child self-control. Specifically, less predictable maternal signals to the infant during the first postnatal months were associated with poor self-control at the end of the first year of life. The correlation between unpredictable patterns of maternal signals and self-control persisted to school age in the cohort (Irvine) that was followed long-term. The consistency of these findings across two distinct demographic and cultural cohorts substantiates the finding that, in addition to the quality of maternal care, patterns and specifically unpredictable sequences of maternal care behaviors influence the maturation of circuits in the developing brain involved in the regulation of emotion and behavior, in a manner indicative of vulnerability to subsequent psychopathology.