Drawing from Uses and Gratifications Theory (UGT), this study explored the interplay between personality traits (online disinhibition, moral disengagement, narcissism, and aggression) and cyberbullying perpetration motives (entertainment, revenge, harm, and dominance) through structural equation modeling. The participants were a convenience sample of 598 cyber bully-victims who were Turkish university students (229 females, 362 males, and seven unknown). The findings empirically supported UGT for conceptualization of cyberbullying perpetration. Almost half of the participants (49.7%) cyberbullied someone twice or more during the preceding 6 months, and males cyberbullied others significantly more than females. In terms of the structural interrelationships, (a) online disinhibition was the only personality trait related to cyberbullying others for entertainment; (b) moral disengagement and aggression were the two variables associated with the revenge motive of cyberbullying perpetration; (c) although online disinhibition was negatively related to cyberbullying others for harm, moral disengagement and aggression were positively linked to harm; and (d) moral disengagement and narcissism were the two personality trait variables associated with the dominance motive of cyberbullying perpetration. Results imply that UGT offers a new understanding about cyberbullying perpetration to researchers, theorists, and practitioners. Personality traits play an important role in cyberbullying perpetration motives and behaviors. Thus, personality traits should be considered in prevention and intervention efforts against cyberbullying. The earlier the personality characteristics of the young individuals are identified, the earlier they can be prevented from engaging in cyberbullying perpetration. Also, sports activities, social events, competitive contests, or leisure and recreational activities offered by university managements can help the university youth to keep away from cyberbullying perpetration and to satisfy motives in more appropriate ways.