In order to improve the removal ability of chitosan (CS) to heavy metal ions, in this study, rich amino-functionalized CS electrospun membranes have been prepared. During the efficient synthesis, poly (glycidyl methacrylate) (PGMA) and polyethylenimine (PEI) were sequentially grafted on the surface of CS electrospun membrane. The success of introduction of amino-group on the CS were confirmed by X-ray diffractometer (XRD), attenuated total reflection-fourier transform infrared (ATR-FTIR), and X-ray photoelectron spectroscopy (XPS). The ability of remove heavy metal ions (Cr(VI), Cu(II) and Co(II)) of the as-prepared membrane (CS-PGMA-PEI) was investigated. The adsorption equilibrium of the heavy metal ion solutions was rapidly established in 60 min. Adsorption kinetics analysis reveals that the adsorption process of CS-PGMA-PEI electrospun membrane was dominated by a Pseudo-second-order model. Its adsorption isotherm can be described by the Langmuir model. The maximum adsorption capacities calculated by Langmuir model were 138.96, 69.27 and 68.31 mg g(-1) for Cr (VI), Cu(II) and Co(II), respectively. The adsorption ability of CS-PGMA-PEI electrospun membrane toward metal ions was found in an order of Cr(VI) > Cu(II) > Co(II). CS-PGMA-PEI membrane also exhibited a good reproducibility and stability. Our study may provide a way to synthesize membranes for water purification.