The Upper Moulouya region, including the Mibladen (M) and Zaïda (Z) mines, is one of the highest lead (Pb) deposit areas in Morocco. These mines, abandoned without any measure of rehabilitation, constitute the main source of soil pollution by Metallic Trace Elements (MTEs) accumulation in the region. In this study, two greenhouse phytoremediation experiments (for the Mibladen and Zaida sites) were set up using Italian ryegrass (Lolium multiflorum) specie to assess its capacity and ability to remediate soils contaminated by zinc (Zn), cadmium (Cd), copper (Cu), and Pb. For both experiments, various factors including (i) three substrates (waste treatment [Wt]; clay uncovering [Cun]; and unpolluted control soil [Ucs]) and (ii) three treatments (no treatment, treatment with organic matter, and treatment with chemical fertilizers) were studied. The results before planting indicated that Wt substrates had poorer physicochemical properties than those of Cun, thus they are the most exposed to the degradation phenomena. This is confirmed by pollution index (PI) results that revealed the trend of PI (Z Wt)> PI (M wt)> PI (M Cun)> PI (Z Cun)> PI (Z Ucs)> PI (M Ucs). The results of experiments indicated that ryegrass crops can grow on substrates contaminated with MTEs. Depending on the applied fertilizers, available metals, and the type of soil, the phytoremediation results showed that L. multiflorum can tolerate, hyperaccumulate, and translocate MTEs from polluted substrates. Our findings suggest that this plant can be a solution for remediating alkaline soils polluted by Cd, Pb, Zn, and Cu in Mediterranean conditions.