Prolonged exposure to landfill leachate can weaken the impermeability of liner systems, leading to leachate leakage and the contamination of surrounding soil and water. To improve loess impermeability to enable its use as a liner material, this study uses synthetic landfill leachate to investigate its effects on loess permeability via a series of laboratory tests. This study focused on the influence of varying dosages of calcium lignosulfonate (CLS) on loess permeability, along with its capacity to adsorb and immobilize heavy metal ions. Microscale characterization techniques, including Zeta potential analysis, X-ray fluorescence spectroscopy (XRF), and scanning electron microscopy (SEM), were employed to investigate the impermeability mechanisms of CLS-modified loess and its adsorption behavior toward heavy metals. The results indicate that the permeability coefficient of loess decreases significantly with increasing compaction, while higher leachate concentrations lead to a notable increase in permeability. At a compaction degree of 0.90, the permeability coefficient was reduced to 8 × 10
−8 cm/s. In contrast, under conditions of maximum leachate concentration, the permeability coefficient rose markedly to 1.5 × 10
−4 cm/s. Additionally, increasing the dosage of the compacted loess stabilizer (CLS) effectively reduced the permeability coefficient of the modified loess to 7.1 × 10
−5 cm/s, indicating improved impermeability and enhanced resistance to contaminant migration. With the prolonged infiltration time of landfill leachate, the removal efficiency of Pb
2+ gradually decreases and stabilizes, while the Pb
2+ removal efficiency of the modified loess increased by approximately 40%. CLS-modified loess, through multiple mechanisms, reduces the fluid flow pathways and enhances its adsorption capacity for Pb
2+, thereby improving the soil’s protection against heavy metal contamination. While these results demonstrate the potential of CLS-modified loess as a sustainable landfill liner material, the findings are based on controlled laboratory conditions with Pb
2+ as the sole target contaminant. Future work should evaluate long-term performance under field conditions, including seasonal wetting–drying and freeze–thaw cycles, and investigate multi-metal systems to validate the broader applicability of this modification technique.
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