© 2019 The hydraulic and chemical compatibility of a geosynthetic clay liner (GCL), containing powdered Na-bentonite, was evaluated against artificial acid rock drainage (ARD) in terms of the swell index, hydraulic conductivity and heavy metal retention. Six artificial ARDs with an approximate pH of 3 and different metal concentrations (electrical conductivity, EC, ranging between 75 and 1000 mS/m; ionic strength ranging between 8 and 400 mM) were used in the experiments. The results of free swelling tests showed that high metal concentrations (EC higher than 70 mS/m) negatively impact the swell volume by lowering it. The hydraulic conductivity of the GCL permeated with distilled water was 1.2 × 10−11 m/s, falling in the range of 7.9 × 10−12 to 1.1 × 10−10 m/s when prehydrated with distilled water and permeated with ARDs. The ion exchange and metal precipitation appeared to be the main mechanisms controlling the metal attenuation on the bentonite. The ion exchange mechanism starts with the release of Na from the bentonite and the sorption of the bi- and tri-metals present in the ARDs onto the bentonite. After the depletion of Na, the ion exchange reaction proceeds with the desorption of Ca and Mg from the bentonite and the sorption of cations present in the ARDs onto the bentonite layers. The depletion of Na from the bentonite and the subsequent release of Ca and Mg correlate to the sudden drop in pH and a gradual increase or equilibration of the hydraulic conductivity. It is possible to say that, after this point, hydraulic and chemical equilibrium is reached. From the overall results, the tested GCL showed acceptably low hydraulic conductivity and the potential to attenuate heavy metals present in ARDs.