This paper analyses the effect of environmental changes observed in the 20th century on hydrology and water management in the southern Pyrenees, in terms of land use and climate. Moreover, a projected water-resource scenario for the 21st century is presented and discussed. Our results demonstrate that changes in precipitation, temperature, and snow accumulation, together with an increase in vegetation density in headwater regions, have led to a marked reduction in water availability in the region. Water resource managers have introduced major changes to dam operations to meet increasing water demand for irrigation purposes in lowland areas. Climatic and land-cover scenarios for the next century indicate that the sustainability of the equilibrium between available resources and water demand will be seriously threatened. These changes predicted for the Pyrenees may be representative of the changes that will occur within many other Mediterranean mountain sectors with similar climatic and socio-economic conditions.