The aim of this study is to analyse the connection between bullying and the dichotomy satisfaction-frustration of the basic psychological needs in adolescents. A total of 1845 students from Secondary Education (928 boys and 917 girls), and Baccalaureate-Year 1 (n = 278), aged between 12 and 17 (M = 14.51, SD = 1.55), from 16 schools of four Spanish provinces participate in the study. Students complete the Psychological Needs Satisfaction-Frustration Scale and the subscale Victimization from the European Bullying Intervention Project Questionnaire concerning three subjects: Mathematics, Spanish Language and Literature, and Physical Education. Results from the structural equation analysis reflect that victimization negatively predicts the satisfaction of the three basic psychological needs of competence, relatedness and autonomy, and positively the frustration of them in the three subjects. These results show the importance of creating educative contexts oriented to promote an increase of the students’ basic psychological needs of autonomy, relatedness and competence to prevent and/or lessen the possible effects of bullying in their victims.