Numerous studies have examined arsenic adsorption on varying adsorbents including iron oxides, aluminum hydroxides, alumina, and carbon as a means of arsenic removal in drinking water treatments. The objectives of this study were to evaluate the effect of magnetite particle size on the adsorption and desorption behavior of arsenite and arsenate, and to investigate the competitive adsorption between natural organic matter (NOM) and arsenic. Increases in adsorption maximum capacities for arsenite and arsenate were observed with decreasing magnetite particle size. Arsenic desorption is hysteretic, more so with the smaller nanoparticles. Such desorption hysteresis might result from a higher arsenic affinity for magnetite nanoparticles. In the presence of NOM, substantial decrease in arsenic sorption to magnetite nanoparticles was observed. It would be beneficial to thoroughly investigate adsorption and desorption of arsenic on magnetite nanoparticles for further practical purposes.