Ecosystem services (ESs) are increasingly included into decision-making to achieve Sustainable Development Goals (SDGs). Although both concepts consider the interactions between humans and the environment, spatial relationships between ESs and sustainability have been rarely addressed. Therefore, this study aims at analyzing spatial congruencies and mismatches between ESs and sustainability in the greater Alpine region. Using hot spot and overlap analyses, we overlaid maps of supply, demand and flow of eight key ESs with the spatial distribution of sustainability based on 24 indicators. Our results reveal that, in most cases, supply of and demand for ESs are greatly dislocated. These mismatches are reflected also in the spatial distribution of sustainability. In contrast to ES demand hot spots, supply hot spots are generally characterized by high sustainability levels, especially in relation to the environment. However, due to discrepancies in the social and economic dimensions, it cannot be assumed that ES supply hot spots always correspond to high sustainability. Hence, using ES indicators for measuring sustainability provides rather limited insights. We conclude that both concepts should be applied in a complementary way to maximize ecological, social and economic benefits in land management and planning processes.