Mobile phone addiction is a universal phenomenon that has attracted a lot of attention in recent years. Previous researches revealed a significant relation between adverse childhood experiences (ACEs) and addiction. This study further investigated the association between ACEs and mobile phone addiction, and the mediating effects of attachment styles and interpersonal relationships. The cross-sectional design and multiple questionnaires, namely, the Revised Adverse Childhood Experience Questionnaire, the Mobile Phone Addiction Index, the Revised Adult Attachment Scale (AAS), and the Interpersonal Relationship Comprehensive Diagnostic Scale (IRCDS) were used in the sample of 345 university students. Correlation analysis revealed that adverse childhood experience, attachment anxiety, attachment avoidance, interpersonal relationship, and mobile phone addiction were significantly positively correlated with each other. Results of regression analysis showed that attachment style and interpersonal relationship played multiple mediation roles in the association between adverse childhood experience and mobile phone addiction. That is, (1) adverse childhood experience was positively related to mobile phone addiction, (2) both attachment anxiety and interpersonal relationship played partial and parallel mediating roles between adverse childhood experience and mobile phone addiction, and (3) attachment anxiety/avoidance and interpersonal relationship mediated the relationship between adverse childhood experience and mobile phone addiction sequentially. These results indicated that mobile phone addiction among college students who had adverse childhood experience can be relieved by way of the remission of attachment anxiety, reduction of attachment avoidance, and improvement of interpersonal relationship.