In response to the changing demands of the U.S. healthcare system and the needs of the nursing profession, the Institute of Medicine, in collaboration with the Robert Wood Johnson Foundation, spearheaded a two-year initiative to develop recommendations for the future of nursing. Discussions of these recommendations within nursing education led to the development of innovative curricula aimed at educating nurses to not only lead change, but also be socially responsible citizens. One educational model that has been developed is academic service-learning, a particular form of experiential education characterized by mutually beneficial campus-community partnerships that emphasize "learning 'with' the community as distinct from learning 'in' the community." This article describes one Catholic university's approach to enhancing nursing curricula by using service-learning pedagogy grounded in Jesuit values to better prepare nursing leaders for healthcare in the twenty-first century. The service-learning experiences that resulted from this initiative provided opportunities to build collaborative relationships in the community, addressed health concerns identified by members of high-needs urban communities, and engaged students in critical reflection focusing on urban challenges and health disparities. The findings suggest that by incorporating the Jesuit values of "cura personalis," reflective practice, and social justice into service-learning opportunities, undergraduate nursing students develop skills to be socially responsible nursing leaders and, at the same time, learn to work collaboratively with communities to address their health needs.