The present study aims to examine the mediating effects of emotion dysregulation in the relationship between psychological maltreatment and non-suicidal self-injury among college students. The participants were 245 freshmen (mean age = 19 years) in a private university in northern Taiwan, and the data was collected by an online questionnaire survey. Questionnaires included Deliberate Self-Harm Inventory, Chinese version of the Childhood Trauma Questionnaire-Short Form, and Difficulties in Emotion Regulation Scale. The results of the present study were as follows: (1) Psychological maltreatment could significantly and positively predict NSSI. (2) Emotional dysregulation could significantly and positively predict NSSI. (3) Psychological maltreatment could significantly and positively predict emotional dysregulation. (4) Emotional dysregulation could partially mediate the relationship between psychological maltreatment and NSSI. The results showed that psychological maltreatment and emotion dysregulation are important factors that may contribute to NSSI among college students. The results indicated that interventions focusing on emotion dysregulation might be helpful for reducing NSSI among college students. Based on the results, the present study offered suggestions for clinical practice and future research.