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The selection of adequate plants that can cope with species that can live in contaminated/degraded and abandoned mining areas is of utmost importance, especially for environmental management and policymakers. In this framework, the use of a fast-growing forestry species, such as Eucalyptus nitens, in the recovery of arsenic (As) from artificially contaminated soils during a long-term experiment was studied. Roots can accumulate to levels ranging between 69.8 and 133 μg g−1 for plants treated with 100 and 200 µg As mL−1, respectively, while leaves between 9.48 μg g−1 (200 As) and 15.9 μg g−1 (100 As) without apparent morphological damage and toxicity symptoms. The C-assimilation machinery performance revealed a gradual impact, as evaluated through some gas exchange parameters such as the net photosynthetic rate (Pn), stomatal conductance to H2O (gs), and transpiration rate (E), usually with the greater impacts at the highest As concentration (200 As), although without significantly impacting the PSII performance. The As effects on the uptake and translocation of Ca, Fe, K, and Zn revealed two contrasting interferences. The first one was associated with Zn, where a moderate antagonism was detected, whereas the second one was related to Fe, where a particular enrichment in leaves was noted under both As treatments. Thus, it seems to exist a synergistic action with an impact on the levels of the photosynthetic pigments in As-treated plant leaves, compared with control plants. E. nitens must be considered as an alternative when phytoremediation processes are put into practice in our country, particularly in areas with cool climatic conditions.