Higher education has an essential role in the promotion of sustainable development. For this to be possible, the use of methodologies in accordance with principles of sustainability must be fostered. This article theoretically analyzes the characteristics that make service-learning an effective tool in education for sustainable development. In order to understand the challenges involved in its implementation in higher education, first of all, the concepts of sustainable development and sustainability are defined. Next, the use of education for sustainable development and curricular sustainability in higher education is contextualized. Finally, the pedagogical proposal of service-learning is addressed and linked to the principles of sustainability in the university environment. To conclude, in relation to prospective applications of service-learning, it is argued that it is an optimal methodology to educate about, for, and from sustainability and that its institutionalization in higher education is highly desirable.