Environmental orderliness can affect both self-control behaviors and creative thinking; however, little research has focused on the moderators of this effect. In this study, we investigated the moderating effect of trait self-control on environmental orderliness, which influences both state self-control behaviors and creative thinking. In Experiment 1, we explored whether trait self-control could moderate the effect of environmental orderliness on state behavioral self-control. The participants have been exposed to an orderly or a disorderly room and asked to complete a breath-holding task to measure self-control. The results showed that low trait self-control participants were more self-controlled in the orderly environment, whereas the self-control of those with high trait self-control was not affected by environmental orderliness. In Experiment 2, the moderating effect of trait self-control on environmental orderliness affecting creative thinking was investigated with a picture priming orderliness and the Alternative Uses Test. As expected, the participants with high trait self-control in the disorderly environment had better creative thinking performance, although there was no difference in the performance of those with low trait self-control between the two environmental orderliness conditions. The results demonstrated that trait self-control could moderate the dual effect of environmental orderliness. The present study sheds light on the effect of environmental orderliness and contributes to the understanding of the common mechanism of the dual effect; also, it has practical implications for the shaping and cultivation of individuals’ self-control behaviors and creative thinking.