Zr-γ-FeOOH nanoparticle adsorbent for As(V) and As(III) removal was prepared by a chemical co-precipitation method. Compared with γ-FeOOH, the addition of Zr enhanced the adsorptive capacities of As(V) and As(III). The maximum adsorptive capacities for As(V) and As(III) were 69.81 and 94.25 mg/g, respectively (rate FeZr =10.5) at pH= 7.0. The adsorption data accorded with Langmuir and Freundlich isotherms. The adsorption of As(III) by Zr- γ-FeOOH was found to be effective in wide pH range of 6–8. Competitive ions hindered the adsorption according to the decreasing sequence phosphate, sulfate, ammonium, chloride, magnesium and calcium. The high adsorptive capability and good performance on other aspects make the Zr-γ- FeOOH nanorods a promissing adsorbent for the removal of As(V) and As(III) from groundwater.