Self-control is important for maintaining good health, acquiring achievement and happiness, and improving environmental adaptability. Trait self-control can affect the processing of emotional conflict in daily life and is associated with successful emotional regulation. In this study, the task functional magnetic resonance imaging (fMRI) technology was adopted to explore the emotion regulation processing and neural mechanism of individuals with different trait self-control levels. The results showed that: (a) Individuals with high self-control experienced the lower intensity of negative emotion when viewing negative emotional pictures than individuals with low self-control, showing spontaneous emotion regulation and significantly increased activity of executive control and emotion regulation networks of the brain; (b) Individuals with low self-control were more sensitive to negative emotion, and their emotion regulation effect under external instructions was better than that of individuals with high self-control. This suggests that individuals with high trait self-control were adept at using proactive control strategies to spontaneously regulate emotional conflict and experienced less emotional conflict accordingly. However, they were less effective than low self-control individuals in resolving emotional conflicts. These findings provide an important basis for our understanding of the nature and neural mechanism of self-control.