Aqueous arsenate [As(V)] was removed using an aluminum-based adsorbent (ABA) and coal mine drainage sludge coated polyurethane (CMDS-PU) prepared using alum and coal mine sludge, respectively. Their As(V) removal efficiencies were compared with each other and granular ferric hydroxide (GFH). The mineralogy and surface chemistry of materials were determined using wavelength dispersive X-ray fluorescence (WD XRF) and Fourier transform infrared spectroscopy (FTIR), respectively. The angle-resolved X-ray photoelectron spectroscopy (AR-XPS) studies confirmed As(V) retention on the adsorbent surfaces. The adsorption kinetics data were fitted to pseudo second-order rate equation. The faster As(V) uptake kinetics of GFH and ABA (GFH > ABA > CMDS-PU) were attributed to their large pore volume and mesoporous nature. Langmuir adsorption capacities of 22, 31 and 10 mg/g, were achieved for GFH, ABA and CMDS-PU, respectively. As(V) adsorption on GFH, ABA and CMDS-PU was endothermic. GFH and ABA were efficient over a wide pH range (3-10). In column studies, GFH, ABA, and CMDS-PU successfully treated 23625, 842, and 158 bed volumes (BVs) and 2094, 6400, and 17 BVs of As(V)-contaminated water with 9.5 and 27 EBCT, respectively (at pH = 6.0, Asi = 600 μg/L). The GFH and ABA have a potential to be used at large-scale aqueous phase As(V) remediation.