This study aimed to examine the unique and joint contributions of behavioral and emotional self-regulation to key but understudied emergent literacy and early social skills, disentangling sex-differentiated paths. The participants were 231 Portuguese preschoolers (50% boys; M[subscript age] = 59.5 months; SD = 8.5) enrolled in 47 classrooms. In the first assessment wave, the children's behavioral self-regulation and receptive vocabulary were individually assessed. The teachers reported on children's emotional self-regulation. In the second assessment wave, individual assessments on children's expressive vocabulary, syntactic knowledge, oral-narrative production, and social problem-solving skills were conducted. The results showed that the children's emergent literacy and early social skills were more related to their behavioral self-regulation than to their emotional self-regulation. Child sex moderated the links between behavioral self-regulation and oral-narrative production skills and the link between emotional self-regulation and early social skills. These findings may have important implications for planning early interventions for developing self-regulation skills.