Naturally occurring layered double hydroxide mineral, brucite (BRU), was compared with hydromagnesite (HYD) and a commercial Mg-rich mineral adsorbent (trade name AQM PalPower M10) to remove antimony (Sb) from synthetic and real wastewaters. The BRU and HYD samples were calcined prior to the experiments. The adsorbents were characterized using X-ray diffraction, X-ray fluorescence, and Fourier transform infrared spectroscopy. Batch adsorption experiments were performed to evaluate the effect of initial pH, Sb concentration, adsorbent dosage, and contact time on Sb removal from synthetic wastewater, mine effluent, and textile industry wastewater. Several isotherm models were applied to describe the experimental results. The Sips model provided the best correlation for the BRU and M10. As for the HYD, three models (Langmuir, Sips, and Redlich–Peterson) fit well to the experimental results. The results showed that the adsorption process in all cases followed the pseudo-second-order kinetics. Overall, the most efficient adsorbent was the BRU, which demonstrated slightly higher experimental maximum adsorption capacity (27.6 mg g-1) than the HYD (27.0 mg g-1) or M10 (21.3 mg g-1) in the batch experiments. Furthermore, the BRU demonstrated also an efficient performance in the continuous removal of Sb from mine effluent in the column mode. Regeneration of adsorbents was found to be more effective under acidic conditions than under alkaline conditions.