Groundwater with high arsenic concentration has widely been found in China. More attention has been paid to economic and efficient arsenic removal technology. Natural siderite, which was abundant and relatively cheap, was used as the main raw material for arsenic adsorption by batch methods. Modified conditions of natural siderite, including temperature and time of calcination and adhesive addition, were carried out for arsenic removal. Results showed that the maximum removal efficiency was reached with the calcination temperature of 350 degrees C for 90 minutes and an adhesive dosage of 10 mg x g(-1). With the ratio of solid to liquid of 0.5 g: 50 mL and the initial concentration of 5 mg x L(-1) for either As(III) or As(V) at 25 degrees C, arsenic concentrations at equilibrium time were lower than 10 microg x L(-1). Characteristics of adsorption kinetics and adsorption isotherm on the optimal modified adsorbent were also evaluated. It was found that the arsenic adsorption kinetics fitted pseudo-second order kinetics equation, and the adsorption achieved equilibrium at about 12 h. The adsorption isotherm could be well described by Langmuir and Freundlich models. The maximum adsorption capacity was 1039 microg x g(-1) for As(III) and 1 026 microg x g(-1) for As(V). Furthermore, X-ray diffraction (XRD), scanning electron microscopy (SEM), and BET method were used to investigate main mechanisms of arsenic removal. Results showed that modified adsorbent had higher specific surface area and contained the spherical coating of Fe(II) and Fe(III) on the surface, in comparison with pristine material, which were believed to contribute to the high adsorption capacity of the modified material. The modified natural siderite appears to be a promising adsorbent that is worthy of further studies and practical application for arsenic removal.