The phytoremediation potential of four crop species cultivated on carbonation lime coming from the sugar industry with water-soluble nickel (Ni) exceeding the Italian legal limit of 10 µg L−1 was assessed. Two autumn–winter species (spinach and canola) were tested with and without the addition of bentonite in a greenhouse experiment in order to overcome prolonged unfavourable weather conditions. Two spring-summer species (sunflower and sorghum) were grown in outdoor boxes. Plant species were selected among crops of interest for phytoremediation and their rotation throughout the year enable to maintain a permanent vegetation cover. Nickel concentration in different plant tissues and the concentrations of soluble and bioavailable Ni in lime were measured. In the greenhouse study, soluble Ni decreased below the legal limit in all the tests, and the combined effect of bentonite and plants reduced Ni in lime mainly in the bioavailable fraction. Spinach and sunflower emerged to be more suitable for phytoextraction than canola and sorghum, because of the higher concentration of the metal in the epigeal portions. The results from the outdoor experiment highlighted that sorghum has a good phytostabilisation potential since its ability to accumulate Ni mainly at the root level and to attract a significant amount of bioavailable Ni in the rhizosphere. This study arose from a real scenario of environmental contamination and investigated the potential of different approaches on the bioremediation of a specific industrial waste product.