The history of uranium mining in Portugal during almost one century has followed international demand peaks of both radium and uranium, which in turn were driven by medical, military, and civil applications. Nowadays, following price drop in the 1980s, mining activities decreased and ceased in 2001. The current challenge is to deal with environmental legacies left by old uranium mines, mainly located in Viseu and Guarda districts. In 2001, based on several radiological surveys carried out, the Portuguese government assumed the remediation costs of abandoned mine areas for environmental safety and public health protection. Detailed environmental and public health risk assessments were performed under the scope of studies both requested by the government and by funded research projects. It was found that the existing risks, due to radiological and chemical exposures to metals and radionuclide's, were particularly high at the old milling facilities and mines where in situ and heap leaching of low-grade ore occurred. The different studies, involving both humans and non-human species from different trophic levels, demonstrated the existence of effects at different levels of biological organization (molecular, cellular, tissues, individuals, and populations) and on ecosystem services. To mitigate the risks, the environmental rehabilitation works at the Urgeiriça mine complex are almost complete, while at Cunha Baixa mine, they are presently in progress. These works and environmental improvements achieved and expected are described herein.