Permeability tests are performed by using the flexible wall permeameter to study the influence of bentonite-HDTMA (hexadecyl trimethyl ammonium bromide) on the permeability performance of Loess as a lining material in the solid waste landfill. Results show, the impermeability of compacted Loess in the middle and lower reaches of the Yellow River in China does not meet the standard requirement as the landfill liner. The permeability of Loess mixed with more than 10% bentonite ratio is less than 1.0 × 10−7 cm·s−1. The permeability of Loess increases slightly after mixing a small amount of HDTMA. The impermeability of Loess mixed with some bentonite-HDTMA ratio still meet the standard requirement. The HDTMA may destroy the soil aggregate structure and increase the soil permeate channel. The SEMs show that the bentonite clay particle can fill the pores between Loess coarse particles and improve the impermeability performance of the material. The digital photos show that HDTMA can effectively resist the development of soil macro-cracks induced by wetting–drying cycles, better for liner to maintain good impermeability. On this basis, the relationship between the hydraulic conductivity of bentonite-HDTMA modified Loess and dry density is constructed. From this study, Loess can be used as a lining material for landfills, when mixed with bentonite/HDTMA at ratios of 10%/0% or 14%/2%.