In this study, industrial wastes, which remain after aluminum extraction from saline slags, were used as adsorbents. The aluminum saline slags were treated under reflux with 2 mol/dm3 aqueous solutions of NaOH, H2SO4, and HCl for 2 h. After separation by filtration, aqueous solutions containing the extracted aluminum and residual wastes were obtained. The wastes were characterized by nitrogen adsorption at -196 °C, X-ray diffraction, scanning electron microscopy, and ammonia pulse chemisorption. The chemical treatment reduced the specific surface area, from 84 to 23 m2/g, and the pore volume, from 0.136 to 0.052 cm3/g, of the saline slag and increased the ammonia-adsorption capacity from 2.84 to 5.22 cm3/g, in the case of acid-treated solids. The materials were applied for the removal of Acid Orange 7 and Acid Blue 80 from aqueous solutions, considering both single and binary systems. The results showed interesting differences in the adsorption capacity between the samples. The saline slag treated with HCl rapidly adsorbed all of the dyes present in solution, whereas the other materials retained between 50 and 70% of the molecules present in solution. The amount of Acid Orange 7 removed by the nontreated material and by the material treated with NaOH increased in the presence of Acid Blue 80, which can be considered as a synergistic behavior. The CO2 adsorption of the solids at several temperatures up to 200 °C was also evaluated under dry conditions. The aluminum saline slag presented an adsorption capacity higher than the rest of treated samples, a behavior that can be explained by the specific sites of adsorption and the textural properties of the solids. The isosteric heats of CO2 adsorption, determined from the Clausius-Clapeyron equation, varied between 1.7 and 26.8 kJ/mol. The wastes should be used as adsorbents for the selective removal of organic contaminants in wastewater treatment.