The effects of calcium on the equilibrium adsorption capacity of As(III) and As(V) onto iron oxide-coated sand (IOCS) and granular ferric hydroxide (GFH) were investigated through batch experiments, rapid small-scale column tests (RSSCT) and kinetics modelling. Batch experiments showed that at calcium concentrations≤20 mg/L, high As(III) and As(V) removal efficiencies by IOCS and GFH are achieved at pH 6. An increase of the calcium concentration to 40 and 80 mg/L reversed this trend, giving higher removal efficiencies at higher pH (8). The adsorption capacities of IOCS and GFH at an equilibrium arsenic concentration of 10 μg/L were found to be between 2.0 and 3.1 mg/g for synthetic water without calcium and between 2.8 and 5.3 mg/g when 80 mg/L of calcium was present at the studied pH values. After 10 hours of filter run in RSSCT, approximately 1000 empty bed volumes, the ratios of C/C_o for As(V) were 26% and 18% for calcium-free model water; and only 1% and 0.2% after addition of 80 mg/L of Ca for filter columns with IOCS and GFH, respectively. The adsorption of As(III) and As(V) onto GFH follows a second-order reaction, with and without addition of calcium. The adsorption of As(III) and As(V) onto IOCS follows a first-order reaction without calcium addition, and moves to the second-reaction-order kinetics when calcium is added. Based on the intraparticle diffusion model, the main controlling mechanism for As(III) adsorption is intraparticle diffusion, while surface diffusion contributes greatly to the adsorption of As(V).