Relatively little is known about the etiology of bullying perpetration and victimization among Macanese adolescents. This study examines the effect of self-control on these behaviors in 365 participants aged between 10 and 17, from two male-only schools (a boarding and a non-boarding school) in Macau. Their bullying perpetration and victimization are measured using the Illinois Bully Scale; their self-control level is assessed by the Self-Control Scale. Bullying perpetration (bullying behaviors and fighting) and victimization are negatively associated with the participants’ self-control level. Participants residing in a school dormitory are found to manifest more bullying behaviors, to exhibit more risk-seeking behaviors, and to be more self-centered than their non-boarding counterparts. Regression analyses indicate that the participants’ living arrangements are significantly related to their involvement in bullying perpetration, whereas their age and their father’s criminal history are significantly associated with their experience of being bullied at school. After controlling for the participants’ demographics, their risk-seeking behavior, self-centeredness, and volatile temper, as indicators for low self-control, are found to have significant effects on their bullying perpetration. These findings provide further support for the importance of self-control in bullying perpetration. Suggestions are offered for fostering adolescents’ self-control as a way to reduce their propensity to engage in bullying perpetration.