This study examined the motivations, or psychological functions, volunteer outcomes and satisfaction of 144 university student mentors who volunteered to work with children in a therapeutic after-school program. This study also explored the predictive value of volunteer mentors' psychological functions, volunteer outcomes, and after-school program quality to volunteer mentors' satisfaction and willingness to volunteer again. For the most part, mentors perceived the after-school programs as being of high quality, particularly in the area of program structure and activities. Mentors' perceptions of the quality of director-child interactions and perceptions of the quality of the after-school classroom teacher-child interactions were less consistent. Both after-school program quality and volunteer outcomes significantly predicted mentors' satisfaction with their service-learning experience in the after-school programs. Specifically, mentors who were more satisfied perceived the after-school program where they volunteered as higher in quality than mentors who were less satisfied. In addition, mentors who were more satisfied experienced more volunteer outcomes as a result of mentoring than mentors who were less satisfied. Program quality and volunteer outcomes together explained 35% of the variance in mentors' satisfaction; thus, these two variables play very important roles in determining how university students experience their service-learning course requirement. Finally, university student mentors who experienced more volunteer outcomes were also more willing to volunteer again than mentors who experienced fewer volunteer outcomes. Implications of these findings for improving after-school program quality and for improving the service-learning experience are discussed.