This study proposes the use of iron and aluminum binary oxide (FeAlO x H y ) to achieve the simultaneous removal of arsenate [As(V)] and F, and the competitive adsorption between As(V) and F are investigated. Iron oxyhydroxide (FeO x H y ) shows a high removal capability towards As(V) but exhibits little efficacy to remove F in systems where both As(V) and F co-exist or for solutions of fluoride alone. The introduction of aluminum oxyhydroxide (AlO x H y ) to FeO x H y within FeAlO x H y enables the removal of F as well as As(V). AlO x H y may simultaneously remove As(V) and F over a wide pH range from 4 to 11; however, the removal of As(V) and F is highly pH dependent and the maximum removal is observed at the weakly acidic pH of 6. The electrostatic force at different pH plays a role, but the dissolution of AlO x H y dominates in the lower removal of As(V) and F by AlO x H y especially at low pH. Furthermore, the removal of As(V) and F by AlO x H y in the co-existing system is lower than that in single pollutant systems due to competitive adsorption effects. The introduction of FeO x H y to AlO x H y significantly alleviates the effect of pH on the removal of As(V) and F by AlO x H y ; moreover, the adverse effects of competitive adsorption between As(V) and F are inhibited to a large extent. In comparison to FeO x H y and AlO x H y , FeAlO x H y shows superior performance in achieving the simultaneous removal of As(V) and F and may be used to treat water containing both As and F.