School entry presents young children with a new set of social and learning demands theorized to be heavily reliant on the development of self-regulation. Children delayed in their development of self-regulation are at heightened risk for problems when they enter school, including difficulty with learning readiness, problematic relationships with teachers and peers, and behavior problems (Blair, 2002). Conceptually, self-regulation is a multi-faceted construct, reflecting the capacity to control impulses, focus and shift attention, and regulate emotion. This set of skills develops rapidly between the ages of 3–7, dependent upon the maturation of the pre-frontal cortex. Although these skills are inter-related developmentally, studies rarely examine them at the same time, raising questions about the degree to which they represent distinct capacities that make unique contributions to school readiness. Collecting multiple measures selected specifically to tap skills relevant to behavioral, emotional, and attentional regulation, the current study provided evidence for a 3-factor structure of self-regulation and documented unique contributions of behavioral, emotional and attentional dimensions to school readiness. In addition, a pilot study suggested that pre-intervention deficits in these self-regulatory skills attenuated response to an innovative time-limited social competence coaching program, although evidence for the malleability of some self-regulatory skills (emotional understanding) also emerged. Implications for developmental models and intervention designs targeting the self-regulatory deficits and school readiness of at-risk children are discussed.