Cyberbullying perpetration has become an international public health concern among adolescents. Based on the general aggression model, the present study sought to examine whether deviant peer affiliation was significantly related to adolescents' cyberbullying perpetration, and whether moral disengagement mediated this association and self-control moderated this mediation process. A total of 2286 Chinese adolescents (M[subscript age] = 13.46, SD = 0.93) completed a series of anonymous questionnaires regarding deviant peer affiliation, cyberbullying perpetration, moral disengagement, and self-control. Results showed that adolescents who interacted with deviant peers were more likely to cyberbully others, which was mediated by moral disengagement. Self-control moderated the association between deviant peer affiliation and moral disengagement and the relationship between moral disengagement and cyberbullying perpetration, but not the relationship between deviant peer affiliation and cyberbullying perpetration. Specifically, compared to high self-control adolescents, low self-control adolescents with high deviant peer affiliation were more likely to develop high moral disengagement and further engage in cyberbullying perpetration. The present study contributes to our understanding of the key mechanisms underlying the association between deviant peer affiliation and adolescents' cyberbullying perpetration.