It has been found that parental psychological control was associated with child problem behaviors. However, not all children who experienced parental psychological control would suffer negative outcomes, indicating that some positive parental behaviors such as parental autonomy support may buffer children from psychological distress. Moreover, previous studies primarily focused on investigating the relationship between parental psychological control and child problem behaviors but rarely explored its mechanism. Available studies have only shown the associations between parenting behaviors and child’s self-control ability, and the associations between child self-control and their emotional and behavioral development. Thus, child’s self-control ability may play a mediating role in associations between parental psychological control and child problem behaviors. Based on Family Systems Theory, The Pressure Buffer Models and General Theory of Crime, the current study aimed to examine the moderating effects of parental autonomy support in the associations between parental psychological control and child externalizing or internalizing problem behaviors and further to explore whether the moderating effects would be mediated by child self-control ability (including inhibitory control and emotional control). Three hundred and forty-three children and their parents from suburb town’s elementary school of Beijing participated in this study. Parental Psychological Control and Autonomy Support Scale (PPCASS), Behavior Rating Inventory of Executive Function (BRIEF) and Youth Self-Report (YSR) were respectively used to assess parental psychological control and autonomy support, child inhibitory control and emotional control, and child problem behaviors. PPCASS and YSR were reported by children in classroom and BRIEF was reported by parents at home. The independent-samples t test, pearson correlation, regression analysis and structural equation model statistical methods were used for data analysis. The result showed: (1) Parents were more likely to use psychological control towards boys than girls. Family socioeconomic status showed significant positive correlations with parental psychological control; (2) Parental psychological control showed significant positive correlations with parental autonomy support, child inhibitory/emotional control, and child internalizing/externalizing problem behaviors. (3) The association between parental psychological control and child internalizing and externalizing problem behaviors were buffered by parental autonomy support. That is, parental psychological control was more strongly associated with child internalizing and externalizing problem behavior in low parental autonomy support than in high parental autonomy support. Additionally, the moderating effects of parental autonomy support between parental psychological control and child internalizing/externalizing problem behaviors were partially mediated by child emotion control, and the moderating effects of parental autonomy support between parental psychological control and child externalizing problem behaviors were partially mediated by child inhibitory control. On the basis of these findings, we concluded that parental autonomy support would moderate the associations between parental psychological aggression and child problem behaviors and further this moderating mechanism was mediated by child self-control. Findings from this study highlight the importance of studying parental negative and positive behavior simultaneously and broaden our understanding of the factors and processes that account for the individual differences in the effects of parental psychological aggression in Chinese families.