European Bison (Bison bonasus) barely escaped extinction in the early 20th century and now only occur in small isolated herds scattered across Central and Eastern Europe. The species’ survival in the wild depends on identifying suitable habitat for establishing bison metapopulations via reintroductions of new herds. We assessed European Bison habitat across the Carpathian Mountains, a stronghold of European Bison and one of the only places where a viable bison metapopulation may be possible. We used maximum entropy models to analyze herd range maps and habitat use data from radio-collared bison to identify key habitat variables and map European Bison habitat across the entire Carpathian ecoregion (210,000 km2). Forest cover (primarily core and perforated forests) and variables linked to human disturbance best predict bison habitat suitability. Bison show no clear preference for particular forest types but prefer managed grasslands over fallow and abandoned fields. Several large, suitable, but currently unoccupied habitat patches exist, particularly in the eastern Carpathians. This available suitable habitat suggests that European Bison have an opportunity to establish a viable Carpathian metapopulation, especially if recent trends of declining human pressure and reforestation of abandoned farmland continue. Our results also confirm the suitability of a proposed Romanian reintroduction site. Establishing the first European Bison metapopulation would be a milestone in efforts to conserve this species in the wild and demonstrate a significant and hopeful step towards conserving large grazers and their ecological roles in human-dominated landscapes across the globe.