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Mentalization theory suggest bidirectional links between a caregiver’s capacity to mentalize their child and emotional regulation in their children. However, there has been little empirical investigation to verify this theory. The bidirectional relationship between caregiver mentalizing and child emotional regulation may be especially important to understand in caregiving contexts where there is greater risk of relationship breakdown or child emotional dysregulation, such as in fostering relationships. This study used a novel time-sequence analysis approach to explore the putative bidirectional relationship between caregiver mentalizing and child emotional regulation in the context of long-term foster care. Existing theories about caregiver mentalizing and child emotional regulation were evaluated and developed by looking at moment-by-moment interactions between a foster carer and a child in her care. The findings of this study gave mixed support for bidirectional relationships between foster carer mentalizing, and child emotional regulation predicted by existing theoretical models. These findings have implications for refining and applying mentalization theory broadly and more specifically in the context of foster care. Furthermore, this study provides a useful example of how time-sequence analysis may be useful for exploring the links between phenomena, such as caregiver mentalizing and child emotional dysregulation, occurring over time in observational data.