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REE have unique properties that are mostly used to manufacture high tech devices. Most REE have geochemical properties that cause them to be typically dispersed and not often found in concentrated and economically exploitable forms, and difficult to separate. The ENVIREE project aims to develop environmentally friendly and efficient methods for their extraction from secondary sources. REE contents of tailings from four legacy mining sites have been obtained by INAA and analysed by 57Fe Mössbauer spectroscopy. REE concentrations in the tailings of Covas and Cumieira are more dependent on the REE contents of the primary ores and the treatment to extract the target metals than on the nano-sized oxides present. The tailings’ size, REE contents and Mössbauer results support the selection of the Covas tailing as the one to be submitted for further steps of REE extraction on the framework of the project.