To advance the understanding about social-cognitive factors related to Chinese adolescents' experience with problematic Internet use (PIU), we examined the associations between social-emotional learning (SEL) competencies (i.e., responsible decision-making, social awareness, self-management, self-awareness, and social relationship) and problematic Internet use (PIU) among 1141 11th grade high school students from Southwest China. Through comparing the latent means of PIU across students with different demographic background (i.e., gender, social-economic status, left-behind status), the study found that male students endorsed higher levels of overall PIU and more problematic time management with Internet use than female students. No latent PIU mean differences were observed across family income and students' left-behind status. Using structural equation modeling (SEM) while controlling for demographic factors, overall SEL competencies were found to have a significantly negative association with PIU. Meanwhile, all five SEL domains were also negatively associated with students' PIU. The findings imply the importance of fostering SEL competencies in preventing PIU among Chinese adolescents. The study provides important practical implications for informing school-based SEL competencies programs for PIU prevention among Chinese youths.