Drawing on self-determination theory and problem-behavior theory, we tested the relation between parental psychological control and adolescents’ problematic mobile phone use, and the sequential mediation effects of basic psychological need experiences (i.e., need frustration and satisfaction) and negative affect in this relation. A total of 4299 Chinese adolescents (46% boys, Mage = 14.48 years, SD = 1.90) participated in this study. We employed structural equation modeling in Mplus 8.0 to test the serial mediation mechanisms. After controlling for adolescents’ gender, age, social desirability scores, and family socioeconomic status in the structural equation model, we found that parental psychological control was positively associated with adolescents’ need frustration and problematic mobile phone use and was negatively associated with their need satisfaction. Need satisfaction and need frustration were negatively and positively associated with negative affect, respectively. However, only need frustration partially mediated the relation between parental psychological control and problematic mobile phone use. Notably, need satisfaction/frustration and negative affect sequentially mediated the relation between parental psychological control and problematic mobile phone use. Additional multiple-group analyses showed some gender and age differences. The present research provides important implications for effective parenting that avoids frustrating adolescents’ basic psychological needs and further prevents their problematic mobile phone use.