As part of the project Rural 3.0: Service-Learning for the Rural Development—RURASL (https://rural.ffzg.unizg.hr/), to ascertain the needs and gaps relevant to implementing service-learning in rural Croatia, we surveyed three target groups: university students, rural community organizations, and potential service-learning beneficiaries. We discovered three main challenges: insufficient human capacities, attributable mostly to difficulty in obtaining funding, which hinders development and implementation of new service-learning projects. Croatian local action groups (LAGs) and rural NGOs were found supportive of rural service-learning. The older population recognizes a great opportunity to get support for basic living needs, and the younger population shows a great interest in engaging university students in improving the tourist and cultural sector. Higher education institutions’ implementation of innovative service-learning will improve the quality of education for sustainable development and promote university–community partnerships in rural areas.