The mining industry has left an important legacy of inadequately abandoned tailing storage facilities (TSFs) in the north-central area of Chile, and they may pose environmental risks. The Chilean government has recently established new regulations governing the closure of TSFs, and these regulations favor the use of environmentally sustainable technologies. Among these technologies is phytostabilization, which can use native plant species that may also have economic and/or subsistence value. Phytostabilization programs based on sustainably maintained native species could also contribute to the conservation of both local flora and regional ecosystems in north-central Chile. The main objective of this study was to use the Coquimbo region as a case study area to look for added economic value from native plant species that have spontaneously colonized abandoned TSFs and to look for other species that, given their ecological characteristics, may be established on post-operational TSFs by phytostabilization. A review of technical, scientific and ethnobotanic literature on traditional uses and recently discovered uses of selected plant species was performed. The results showed that 68 spontaneously colonizing phytostabilization species have at least one known use, while 420 species with potential for use in phytostabilization (28% of the regional native flora) have various uses. Ornamentation, cattle forage, mellipherous, medicine, crafts and phytochemicals are the main uses identified for the local native flora. Most of the identified species are endemic to Chile (69%). These species are therefore a very valuable phytogenetic resource that can be used in the rehabilitation of massive mine wastes. This unique resource could be lost if these species are not identified and studied in the near future.