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Large ultramafic areas exist in Albania, which could be suitable for phytomining with native Alyssum murale. We undertook a five-year field experiment on an ultramafic Vertisol, aimed at optimizing a low-cost Ni-phytoextraction crop of A. murale which is adapted to the Balkans. The following aspects were studied on 18-m² plots in natural conditions: the effect of (i) plant phenology and element distribution, (ii) plant nutrition and fertilization, (iii) plant cover and weed control and (iv), planting technique (natural cover vs. sown crop). The optimal harvest time was set at the mid-flowering stage when Ni concentration and biomass yield were highest. The application of N, P, and K fertilizers, and especially a split 100-kg ha⁻¹ N application, increased the density of A. murale against all other species. It significantly increased shoot yield, without reducing Ni concentration. In natural stands, the control of graminaceous weeds …