The devastating consequences of cyberbullying during adolescence justify the relevance of obtaining empirical evidence on the factors that may cause participation in its distinct roles. The goal of this study was to analyze the predictive capacity of aggressiveness (physical aggression, verbal aggression, anger, and hostility) and emotional intelligence (attention, understanding, and emotional regulation) with respect to being a victim, aggressor or victim–aggressor of cyberbullying during adolescence. The Screening for Peer Bullying, the Aggressiveness Questionnaire and the Trait Meta-Mood Scale-24 were administered to a sample of 1102 Spanish secondary education students, aged 12 to 18. In general, results revealed a higher probability of being a victim, aggressor or victim–aggressor as physical aggressiveness and anger increased. On the other hand, results revealed a low probability of being a victim, aggressor or victim–aggressor as emotional understanding and emotional regulation increased. These findings highlight the importance of considering said variables when creating prevention programs to stop or reduce the social and educational issue of cyberbullying during adolescence.