Recent works show that modified natural zeolites improve the remotion of anionic or non-polar organic pollutants from water. In this work the arsenic sorption from aqueous solutions onto clinoptilolite–heulandite rich tuffs modified with lanthanum, hexadecyltrimethylammonium or iron was investigated considering the arsenic chemical species and the pH of the arsenic solutions. Clinoptilolite–heulandite rich tuffs were characterized by scanning electron microscopy and X-ray diffraction analysis. The elemental composition of the zeolitic samples was also determined. According to the Langmuir isotherm model the arsenic (V) sorption capacity of the zeolites was 75.4 μg As/g at pH 3, 3.9 μg As/g at pH 5 and 53.6 μg As/g at pH 6, for the lanthanum, HDTMA and iron modified clinoptilolite–heulandite rich tuff from Chihuahua (México), respectively. In general, the results suggested that the arsenic retention depends on the precedence of zeolitic material, the nature of arsenic chemical species, pH as well as the characteristics of modified natural zeolites. In this work the arsenic adsorption mechanisms are also discussed.