Arsenic (As) poses a tremendous threat to human health due to exposure through arsenic-contaminated drinking water and/or food. We aimed to develop organically modified clay adsorbents for the removal of As from aqueous solution. We modified a smectite sample using three organic agents, namely hexadecyl trimethylammonium (HDTMA), chitosan and citric acid, and characterized the products using X-ray diffraction, infrared spectroscopy, and scanning electron microscopy techniques. The characterization techniques suggested successful organic modifications of the smectite sample. The surfactant-modified smectite was the most efficient (66.9%) As removing adsorbent with a maximum adsorption capacity of 473.2 μg g-1. Kinetic study showed that the adsorbents reached As adsorption equilibrium within 3 h, and the data fitted reasonably well to power function and simple Elovich equations (R2 > 0.89). The adsorption data were explained well by the Freundlich and Sips isothermal models. The surfactant-modified and chitosan-grafted organoclays adsorbed As by electrostatic attraction and anion exchange, whereas the citric acid activated smectite followed ligand exchange and simple anion exchange mechanisms. This study thus demonstrated the potential of surfactant-modified clays in removing As from contaminated waters.