College students face multiple challenges such as distraction and learning pressure in the course of their intense academic life. This study investigated whether calligraphy training, which originates from traditional culture, can serve as an effective intervention mechanism to improve college students’ emotional regulation and mental health. The study utilized a pre- and post-test experimental design, and 106 college students were exposed to a 40-day calligraphy training intervention. The mental health and emotion assessments of the two groups of college students were conducted using the Mental Health Quality Questionnaire for College Students and the Emotion Regulation Scale, and the mediating effect of emotion regulation on mental health in calligraphy training was analyzed by the SPSS macro program PROCESS. The results of the study showed that calligraphy training could significantly improve the overall mental health quality and emotion regulation ability of college students, among which the effect of line calligraphy training in promoting students’ psychological relaxation was more significant. The mediating effect analysis further revealed that calligraphy training also had an indirect positive effect on college students’ psychological health by enhancing students’ cognitive reappraisal and reducing expressive inhibition. This paper provides a reference for developing scientific psychological intervention programs for college students.