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This study aimed to assess the mental health problems of college students and to explore whether mentalization and psychological flexibility are significantly associated with the mental health of college students. The mental health of 14,481 undergraduate students was evaluated using the Generalized Anxiety Disorder 7 and Patient Health Questionnaire-9. Mentalization was assessed using the Reflective Functioning Questionnaire, and psychological flexibility was evaluated using the Acceptance and Action Questionnaire-II and Cognitive Fusion Questionnaire. Mental health was measured using the Patient Health Questionnaire-9 and the 7-item Generalized Anxiety Disorder Scale. Multivariate and linear regression analyses were employed to examine the relationships among mentalization, psychological flexibility, and the mental health of college students. The Bootstrap procedure was used to explore the mediating role of psychological flexibility in mentalization and mental health. The mental health status of the college students revealed that mentalization and psychological flexibility were significantly related to anxiety and depression in college students. Age, gender, status of the only child, and marital status of parents were significantly related to anxiety and depression of college students. In addition, left-behind children were associated with depression, and higher hypermentalization scores were associated with higher anxiety and depression scores, indicating more severe anxiety and depression. Higher hypomentalization scores are associated with higher depression scores, indicating more severe depression. Psychological flexibility (cognitive fusion, acceptance, and action) partially mediated the relationship between hypermentalization and anxiety/depression scores, and a masking effect was observed in the relationship between hypomentalization and anxiety/depression scores. Anxiety and depression of college students are significantly related to mentalization and psychological flexibility.