Layered double hydroxides (LDHs) are very promising adsorbents for the removal of anionic pollutants from water. However, the low adsorption efficiency and recycling difficulty of conventional LDH powders are obstacles to practical applications. Herein, a novel Zn/Fe-LDH composite sponge was successfully fabricated using a simple in-situ hydrothermal method. Characterization studies revealed that the composite sponge contained flower-like Zn/Fe LDH microspheres uniformly dispersed throughout a poly vinyl alcohol (PVA) sponge matrix. The specific surface area of the Zn/Fe-LDH composite sponge was 42.5 m(2) g(-1), approximately 5 times higher than the pristine PVA sponge (8.9 m(2) g(-1)). Adsorption experiments revealed that Zn/Fe-LDH composite sponge exhibited a much higher adsorption ability for As(V) anions and methyl orange (MO) compared with a Zn/Fe-LDH powder or the pristine PVA sponge. The maximum adsorption capacity for As(V) was found to be 85.7 mg g(-1). Furthermore, the Zn/Fe-LDH composite sponge showed high thermal stability, good mechanical stability and easy recoverability, thereby allowing reuse. Results guide the development of improved, low cost water treatment materials.