The present study investigated the relationships between self-efficacy, attentional control, and procrastination by examining whether and how the five dimensions of attentional control, including inhibitory control, attention shifting, task persistence, attention concentration, and attention distribution, would work as significant mediators to explain the association between self-efficacy and procrastination. A sample of 293 Chinese adults participated in the study. Mediation analyses suggested that task persistence, attention concentration, and attention distribution played a significant mediating role in the association between self-efficacy and procrastination. Specifically, we found that individuals with higher self-efficacy were more capable of directing their concentration to their tasks and persisting over time, making them less prone to procrastinate. On the other hand, individuals with higher self-efficacy were also more likely to distribute their attention across multiple tasks, which was related to an elevated likelihood of procrastination. The current study revealed a double-edged effect of self-efficacy on procrastination and emphasized the significance of attentional control in understanding the working mechanisms underlying the association between self-efficacy and procrastination, which can provide valuable insights for designing effective interventions to avoid procrastination.