Pyrite (FeS2) is usually a waste from complex sulfide ores. Yet, it may be a remediation additive for calcareous soils deficient in iron (Fe) and other micronutrients such as copper (Cu), zinc (Zn), and manganese (Mn). In this study, leaching experiments were conducted under laboratory conditions and a 30-day pot trial (with wheat) to evaluate the effect of applying different amounts of pyritic tailings on micronutrient and heavy-metal concentrations in a calcareous soil and on crop growth (dry-matter production). The application of pyritic tailings to the calcareous soils improved the levels of Fe, Cu, Zn, and Mn, and dry-matter biomass of wheat also significantly increased. The heavy-metal contents in soil and plant were well below the permissible limit for soil and plants.