Habitat destruction reduces biodiversity and affects ecosystem functioning, putting at risk the provision of ecosystem services (ESs) essential for human well-being. Ecological restoration using native species with multiple uses may offer a long-term supply of natural resources for vulnerable human populations. We selected priority areas for restoration in the Brazilian Seasonally Dry Tropical Forest (Caatinga), targeting areas with high ES demand but low supply. We estimated the supply and demand for three ESs: (1) food/medicine, (2) wood production, and (3) pollination. We estimated ES supply using maps of the potential geographical distribution of 194 native plant species used by the local population as a means of livelihood. For ES demand, we used maps of population density, rural municipalities, wood productivity, and crops dependent on pollination. We used a large-scale prioritization tool (Zonation) to select two scenarios for each ES: (1) ES supply-only and (2) ES supply + ES demand, selecting only nonvegetated areas. To select priority areas, where the potential occurrence of species (ES supply) corresponds to areas of high demand for the same services, we overlapped the maps of the two scenarios for each ES. The highest percentage of scenario overlap occurred for food/medicine ES (45%), whereas pollination showed the lowest percentage of overlap (10%), indicating little similarity between potential ES supply and demand areas. Our study shows the importance of including ES in ecological restoration opportunities, taking into account the vulnerable human population in dry regions and their demand for natural resources.