Advanced modified polyacrylonitrile (PAN) membrane with high adsorption property for heavy metal ions was designed and fabricated for the first time. The introduced diazoresin-ethylenediaminetetraacetic acid (DR-EDTA) layer could effectively absorb the metal ion, such as Cu2+, Pb2+, Hg2+ in the waste water. The effects of layers, metal ion concentration, pH, temperature and cycle time were investigated. The results showed that the adsorption isotherms for Cu2+ were well fitted by Langmuir model. The maximum adsorption capacity of the modified membrane for Cu2+ was approximately 47.6 mg/g. In addition, the prepared PAN-(DR-EDTA)3 membrane could be regenerated more than 720 h based on their adsorption/desorption cycles. The results demonstrated that the modified PAN membrane could be used as effective adsorbents for heavy metal removal from waste water.