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Acid mine drainage (AMD) is one of the main environmental problems associated with mining activity, whether the mine is operational or abandoned. In this work, several precipitates from this mine drainage generated by the oxidation of sulfide minerals, when exposed to weathering, were used as adsorbents. Such AMD precipitates from abandoned Portuguese mines (AGO, AGO-1, CF, and V9) were compared with two raw materials from Morocco (ClayMA and pyrophyllite) in terms of their efficiency in wastewater treatment. Different analytical techniques, such as XRD diffraction (XRD), Fourier Transform Infrared spectroscopy (FTIR), N2 adsorption isotherms, and Scanning Electron Microscopy (SEM) with Energy Dispersive X-ray (EDX) were used to characterize these natural materials. The adsorption properties were studied by optimizing different experimental factors, such as type of adsorbent, adsorbent mass, and dye concentration by the Box–Behnken Design model, using methylene blue (MB) and crystal violet (CV) compounds as organic pollutants. The obtained kinetic data were examined using the pseudo-first and pseudo-second order equations, and the equilibrium adsorption data were studied using the Freundlich and Langmuir models. The adsorption behavior of the different adsorbents was perfectly fitted by the pseudo-second order kinetic model and the Langmuir isotherm. The most efficient adsorbent for both dyes was AGO-1 due to the presence of the cellulose molecules, with qm equal to 40.5 and 16.0 mg/g for CV and MB, respectively. This study confirms the possibility of employing AMD precipitates to adsorb organic pollutants in water, providing valuable information for developing future affordable solutions to reduce the wastes associated with mining activity.