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Ample research demonstrates that parents’ experience-based mental representations of attachment—cognitive models of close relationships—relate to their children’s social-emotional development. However, no research to date has examined how parents’ attachment representations relate to another crucial domain of children’s development: brain development. The present study is the first to integrate the separate literatures on attachment and developmental social cognitive neuroscience to examine the link between mothers’ attachment representations and 3- to 8-year-old children’s brain structure. We hypothesized that mothers’ attachment representations would relate to individual differences in children’s brain structures involved in stress regulation—specifically, amygdala and hippocampal volumes—in part via mothers’ responses to children’s distress. We assessed 52 mothers’ attachment representations (secure base script knowledge on the Attachment Script Assessment and self-reported attachment avoidance and anxiety on the Experiences in Close Relationships scale) and children’s brain structure. Mothers’ secure base script knowledge was significantly related to children’s smaller left amygdala volume but was unrelated to hippocampal volume; we found no indirect links via maternal responses to children’s distress. Exploratory analyses showed associations between mothers’ attachment representations and white matter and thalamus volumes. Together, these preliminary results suggest that mothers’ attachment representations may be linked to the development of children’s neural circuitry related to stress regulation.