Very often, in-situ soil does not meet the requirements for landfill barriers; therefore, it is necessary to purchase the material from quarries. An increasing number of by-products have been proposed as alternative landfill barrier materials. The present study investigated the performance of two soils of Central Italy (alluvial and volcanic soils) with an organosolv lignin (sulfur-free lignin (SFL)), a widespread by-product in the world. Laboratory investigations indicated that the volcanic soil mixed with 10% in weight of lignin did not reach the permeability value required for landfill bottom liners, also showing high compressibility. On the contrary, the addition of 20% to 30% lignin to the alluvial soil reached the permeability value recommended for the top-sealing layer of landfills: scanning electron microscope analysis indicated that the improvement was due mainly to the physical binding. Large-scale investigations should be carried out to evaluate the long-term performance of the mixtures. The increasing production of organosolv lignin worldwide gives this by-product the opportunity to be used as an additive for the realization of the top-sealing layer. The approach can save the consumption of raw materials (clayey soils from quarries), giving lignin a potential new field of application and recovering in-situ soils.