Agrocybe cylindracea substrate-Fe3O4 (ACS-Fe3O4), a Fe3O4 nanoparticle coated biomaterial derived from agriculture waste from mushroom cultivating, was investigated to remove the hexavalent chromium ions (Cr(VI)) from aqueous solution. After modification, the material surface become uneven with polyporous and crinkly structure, improving the Cr-accommodation ability in a sound manner. Optimized by Taguchi method, Cr(VI) removal efficiency was up to 73.88% with 240min, 40°C, pH 3, Cr(VI) at 200 mg L-1, dosage at 12 g L-1, rpm at 200. The efficient ions removal was due to the combined effect of adsorption and redox. The effect of storage time of the material on Cr(VI) removal was small which enhanced its value in practical application. Results indicated that metal removal was mainly dependent on solution concentration, adsorbent dosage and treatment time. The experimental data obtained was successfully fitted with Langmuir isotherm model. Thermodynamic study indicated the endothermic nature of the process. The results confirmed that ACS-Fe3O4 as novel material, with the ability for long-term preservation, could be applied for heavy metal remove from wastewater as well as waste cycling.