Dual language use is thought to afford certain cognitive advantages to bilingual children and may function as an additional resource to help low-income Mexican-American children achieve academically. Emotion regulation and executive functioning (e.g., inhibition) have been found to be particularly important in studies investigating pathways to early academic achievement. Understanding how we can capitalize on children’s bilingual abilities to strengthen their executive functioning and emotion regulation, or to offset problems in these domains, may be important to promote better educational outcomes and inform policy. Thus, the current study investigated the relation between emerging bilingualism, inhibition, emotion regulation, and academic achievement across early childhood in sample of 322 low-income, Mexican-American children. Data were collected in a laboratory space at child ages 36-, 54-, and 72-months. Bilingualism was indexed as the interaction of Spanish and English vocabulary, and a mediated moderation model was examined. Results provided further evidence that inhibition positively predicts academic achievement during early childhood. Greater Spanish language vocabulary indirectly predicted academic achievement while controlling for English language vocabulary, suggesting that children from immigrant families may benefit from maintaining their Spanish language abilities as they begin to immerse themselves in an English-speaking classroom. Advancing our understanding of the development of self-regulatory abilities within bilingual, immigrant populations could have significant implications for educational policy.