This paper reports zirconium oxide-coated sand preparation, characterization by SEM, EDX, XRD, FT-IR and thermoanalytical techniques, and use as an adsorbent for the removal of most toxic form of arsenic, As(III), from aqueous solution in both batch and column methods. Batch experimental parameters such as contact time, concentration, dose of adsorbent, pH of As(III) solution and temperature were optimized. The adsorption data was fitted to Langmuir, Freundlich, Temkin and Dubinin-Radushkevich isotherms at 303, 308 and 313 K. The maximum Langmuir monolayer adsorption capacity was found to be 136.98 μg/g at 313 K. Values of ΔH°, ΔG° and ΔS° were found to be −12.90, −8.74 to –8.28 and 0.014 kJ/mol, suggesting exothermic and spontaneous adsorption process with slight increase in entropy. The adsorption process followed pseudo-second order kinetics and was controlled by film diffusion step. The column studies showed that when flow rate was increased from 3.0 to 5.0 mL/min, the arsenic adsorption capacity of ZrOCS increased from 33.104 to 42.231 μg/g and breakthrough, and exhaustion times got reduced reduced. The results indicated that zirconium oxide-coated sand (ZrOCS) is an excellent adsorbent for the removal of As(III) from water.