A field-based experiment was set up to evaluate the effectiveness of a single application of marble waste sludge (MWS) on chemical immobilization of potentially hazardous trace elements (PHE) within the soil profile of a mine Technosol under natural assisted remediation for 12 years. Results showed that MWS amendment significantly reduced soil acidity and PHE mobility compared to unamended soil, thus improving soil health and plant growth. The amendment application had a sustained acid-neutralizing action, as soil pH remains relatively constant at between 5.8 and 6.4 throughout the entire profile (70 cm depth). In addition to diluting pollutants, the treatment triggered a redistribution of trace elements among the various operationally defined geochemical pools, shifting the PHE speciation from water-soluble forms to fractions associated with carbonates (29% Cd), metal oxides (40–48% Zn, Cd, Cu, and Ni), organic matter (22% Cu and Ni), and insoluble secondary oxidation minerals and residual phases (80–99% As, Cr, Sb, Tl, and Pb), thereby effectively limiting its potential environmental significance. MWS treatment to immobilize PHE in the contaminated mine Technosol was effective and persistent while in the untreated soil metal release is continuing over time.