Although the association of Internet addiction (IA) with self-regulation has been widely observed in previous studies, its variance with age remains poorly understood. Using dual models of self-regulation, we aimed to test the effects of effortful control and impulsivity on IA and to explore the effect of the interaction between age stage and self-regulation on IA. In this study, 4313 students nested in 100 classes were surveyed using the Internet Addiction Test (IAT), the Dual-Modes of Self-Control Scale (DMSC-S) and a demographic questionnaire. Hierarchical generalized linear models (HGLMs) were then used to test our assumptions. The results indicated that the IA prevalence rate among the surveyed adolescents was 10.9%, and IA was found to be negatively related to the effortful control trait and positively related to the impulsivity trait. Compared with primary school students, middle school students were more likely to be Internet addicts; however, the prevalence of IA among college students was comparable to that among middle school students. A slopes-as-outcome model showed that the association between IA and effort control was stronger among junior high school students than among students in other grade levels, but no grade differences were found in the slopes for impulsivity. We integrate our results with the findings of previous studies and discuss possible theoretical implications.