Iron oxide‐coated sand has been demonstrated to be an effective adsorbent material for the removal of arsenic and other metals and metalloids from drinking water and wastewater. In this study, fibrous materials were evaluated for their ability to offer a high specific surface area alternative to sand as the substrate for the iron oxide coating. Four types of fibrous materials, polypropylene, polyester, fiberglass, and cellulose, were evaluated for their ability to retain iron coatings and to remove arsenate. Sand was also evaluated to provide a basis for comparison with previous research. In isotherm experiments, all four fibrous materials showed higher arsenate adsorption densities than iron oxide‐coated sand. Arsenate adsorption densities were highest for iron oxide‐coated fiberglass and cellulose, suggesting that these fibrous materials may offer advantages over iron oxide‐coated sand.