Psychological needs dissatisfaction has been identified as hindering adaptive development, in which autonomy need dissatisfaction, as one core component, may be associated with adolescents’ maladaptive online behaviors. Sporadic research has examined the association between autonomy need dissatisfaction and problematic mobile phone use (PMPU). Boredom proneness and mobile phone gaming were suggested to be linked to this association. This study aimed to examine the mediating effects of boredom proneness and mobile phone gaming in the association between autonomy need dissatisfaction and PMPU. A total of 358 secondary school students completed questionnaires at three waves; autonomy need dissatisfaction was measured in time 1 (T1); boredom proneness and mobile phone gaming were measured one year later (time 2, T2); PMPU was measured two years later (time 3, T3). The structural equation model results showed that T1 autonomy need dissatisfaction not only directly predicted T3 PMPU, but also exerted effects via the mediating role of T2 boredom proneness and the chain mediating role of T2 boredom proneness and T2 mobile phone gaming. These findings reveal the unique role of specific psychological need in engaging PMPU, which provides support to targeted interventions, such that promoting autonomy need satisfaction may be an instrumental procedure to prevent adolescents from addiction-like online behaviors.