An evaluation was made of the use of MgAl-LDH with incorporated nitroprusside as an adsorbent to remove inorganic arsenic (As(III) and As(V)) and organic arsenic (DMA) from aqueous matrices. The material was synthesized by the co-precipitation method at constant pH and was characterized by Raman spectroscopy, infrared spectroscopy, thermogravimetry, X-ray diffraction, and high-resolution transmission electron microscopy, before and after use in the adsorption process. The effects on adsorption of contact time, initial metalloid concentration, and pH were investigated. For an initial concentration of 10 mg L-1 and pH 2.00, the MgAl-LDH with incorporated nitroprusside was only able to adsorb the DMA and As (V) species, with removal percentages of 25.10 and 103.8%, respectively. At pH 6.02 and 12.00, only the inorganic species were adsorbed, with removal percentages of 22.93% and 60.07%, respectively, for As(III), and 89.81% and 71.64%, respectively, for As(V). Application of the Langmuir and Freundlich isotherm models indicated that the features of the adsorption process depended on the pH of the medium and the arsenic species. The results showed that the use of MgAl-LDH with incorporated nitroprusside has potential for the development of techniques for the speciation of arsenic species. (C) 2020 Elsevier Inc. All rights reserved.