High-quality early childhood education and care (ECEC) has a robust and long-term impact on the development of children’s skills and abilities, including self-regulation. While the importance of early self-regulation is acknowledged in national curricular frameworks (Australian Early Years Learning Framework), little is known about practices employed within Australian ECEC settings to support the development of self-regulation; nor do we know how educators understand self-regulation and seek to support its development based on their understanding. The current study sought to observe educators’ practices in support of children’s self-regulation development in six Australian ECEC services identified for their high-quality environments and strong child outcomes. This study also sought to investigate educators’ understandings of self-regulation, its development and their self-reported practices to support self-regulation development of the children in their care. Researcher observations identified the use of diverse practices that theoretical and empirical literature suggest as beneficial for self-regulation, although the pattern of practices differed across services. In interviews and reflection journals educators tended to view self-regulation from a behavioural and deficit perspective. Educators were nuanced in their views of episodic and developmental change, and adopted a comprehensive set of evidence-supported practices to support children’s self-regulation. Taken together, findings provide insight into the discrepancies between definitions, operationalisations and practices for supporting self-regulation, highlighting additional areas of opportunity for ongoing professional learning and continued research—even among high-quality services such as those participating in this research.