While the early years are often regarded as a critical period for establishing and supporting the developmental trajectories of delayed and typically developing children, they also represent a critical time for advanced learners. Yet to support advanced learners, a better understanding of sources and mechanisms of precocious early learning is needed. While there is ample research separately indicating importance of executive functions (EFs) and self-regulation for learning more broadly, it remains unclear whether, which, and to what extent EFs and/or self-regulation might account for the incidence of advanced learning in the prior-to-school years. The current study sought to investigate the EFs and self-regulation of 214 3- to 5-year old preschoolers, to better understand the profile of these abilities amongst advanced compared to non-advanced learners. Measures of self-regulation, EF and academic learning were taken at the start of the final pre-school year, and academic learning was assessed again at the end of the year. Results indicated that consistently advanced learning was predicted by socio-demographic factors (age, socioeconomic context), stronger cognitive development (combined EFs, cognitive aspects of self-regulation), yet lower behavioral self-regulation ratings. Results thus identify a profile of cognitive and behavioral characteristics of advanced early learners, which potentiates early identification and helps to clarify the nature and underpinnings of advanced early learning. It also raises questions about whether lower levels of behavioral self-regulation might constrain learning (e.g., difficulty remaining within the structures and sequences of the situation) or is a hallmark that is promotive of learning (e.g., convergent thinking, creativity).