Consumption of arsenic contaminated water induces and aggravates major health problems in humans. In this report, we have successfully synthesized nanostructured Zr/Cu composite oxide (NZCO) by ultrasonically assisted hydrothermal process for total arsenic sequestration. Various batch experiments were performed with NZCO to determine its adsorption efficacy for As(III) and As(V) species. NZCO demonstrated outstanding performance in removing arsenic species from water with maximum adsorption capacities of 72.25 mg g−1 and 107.5 mg g−1 for As (III) and As (V) respectively under optimized conditions. The adsorption kinetics was closely fitted to pseudo‐second order model and adsorption isotherms were well described by D−R isotherms model. Meanwhile, the adsorption tests performed on naturally occurring ground water samples confirmed the effectiveness of NZCO in remediating total arsenic level below the prescribed limit of WHO‐MCL (0.01 mg L−1). The adsorption mechanisms study exhibits a single‐step arsenic treatment option involving electrostatic interaction and ligand exchange reactions. Various analytical techniques were used to characterize the material. Facile synthesis route combined with excellent performance make NZCO a novel adsorbent in total arsenic removal from drinking water.