Compared with arsenate [As(V)], arsenite [As(III)] is more toxic to human health and more difficult to be removed from aqueous solution. In this study, a novel adsorbent, Zr(IV)-loaded collagen fiber (ZrCF), was prepared, and its adsorption characteristics to As(III) were investigated. It was found that ZrCF can effectively remove As(III) from aqueous solution in the pH range of 9.0-12.0. The maximum adsorption capacity of As(III) by ZrCF reached up to 54.02 mg As/g when the initial concentration of As(III) was 73.00 mg/L at 303 K and pH 11.0. The adsorption isotherms of ZrCF to As(III) were well fitted by the Langmuir-Freundlich equation. The adsorption kinetic experimental data were well described by the pseudo-second-order rate equation, and the calculated adsorption capacities were close to those obtained by experiments. The leakage of zirconium loaded on ZrCF was negligible during adsorption process. Therefore, this study indicates that ZrCF is a promising adsorbent for As(III) removal from aqueous solution.