This study investigated the removal of arsenite (As(III)) and arsenate (As(V)) in aqueous solution using iron-coated pomelo peel (ICPP). Batch adsorption experiments were performed to evaluate the effects of initial pH values (2.0–10), contact time (1–1440 minutes), initial concentration (0.05–5 mg/L) on the As(III) and As(V) removal capacity by ICPP. The Langmuir maximum adsorption capacities of ICPP of As(III) and As(V) at pH 7.0, and 25 °C were 1.51 mg/g and 1.64 mg/g, respectively. The capacities were significantly higher than that of raw pomelo peel (PP) material at the same condition (qmax As(III) = 0.032 mg/g and qmax As(V) = 0.036 mg/g). Adsorption kinetics data fitted well with the Elovich model and the adsorption process quickly reached an equilibrium at around 120 min. The results shows that the As(III) and As(V) adsorption performance of ICPP were much better than that of PP, granular activated carbon (GAC) and many iron-based adsorbents. Thus, ICPP has potential as a filter media for efficiently removing toxic arsenic ions from water.