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Facebook is, nowadays, the most used social networking site worldwide and adolescents are increasingly engaging in this form of communication. Despite increasing attention of researchers to computer-mediated communication, there are few studies using an interpersonal and family relationships perspective on how adolescents relate to the Internet, and particularly to Facebook use. The aim of the present study was to test whether peer alienation mediates the link between parental attachment and problematic Facebook use. To this purpose we used a sample of 761 adolescents (53.7% boys, mean age = 15.8), from the North region of Portugal. We also tested if the mediational model was invariant for boys and girls. The results showed that peer alienation plays a mediating role in the relationship between parental attachment and problematic Facebook use. The mediational models were, however, not invariant for boys and girls. Considering parental attachment, quality of emotional bond directly predicted problematic Facebook use only for boys. These results provide relevant clues for understanding predictors of problematic Facebook use in adolescents and also enlighten psychological intervention, particularly in parental education and school intervention programs.