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Purpose To explore the relationship between self-control, rejection sensitivity, loneliness, and problematic internet use in college students. Patients and Methods A total of 725 college students were investigated using Self-control Scale, Rejection Sensitivity Questionnaire, Loneliness Scale, and Internet Addiction Scale. Results ① Correlation analysis showed that self-control was negatively related to rejection sensitivity, loneliness, and problematic internet use; rejection sensitivity was positively related to loneliness and problematic internet use; loneliness was positively related to problematic internet use. ② Chain mediating effect analysis showed that self-control can not only affect problematic internet use in college students, but also through three indirect paths, as follows: the mediating role of rejection sensitivity and loneliness, the chain mediating roles of rejection sensitivity and loneliness, and the mediating effect size, accounting for 9.76%, 20.73%, and 4.88% of the total effect, respectively. Conclusion Rejection sensitivity and loneliness played a chain mediating role in the relationship between self-control and problematic internet use in college students.