Enhancing college students' learning habits, attitudes, and capacities have been an important research topic in educational psychology. In this study, we designed, implemented, and evaluated a coaching program that integrated mindful agency coaching and motivational interviewing for the development of positive learning dispositions in college students. A randomized control trial embedded mixed-methods design was employed. The quantitative phase with two experimental groups showed that the intervention group (n = 24) showed significant improvement in mindful agency, self-efficacy, learning motivation, and emotional intelligence after the coaching, compared with the control group (n = 30). The qualitative phase with students in the intervention group (n = 15) revealed five themes: Task orientation, motivational management, openness and acceptance, self-awareness and self-regulation, and supporting factors for coaching. Integrated findings demonstrated whether and how coaching could be a promising approach to enhancing college students' various positive dispositions that are essential for them to be mindful, resilient, and self-directed learners.