Chitosan-polyethylene oxide (Cs/PEO) electrospun nanofibers were prepared by electrospinning process in order to remove nickel ions from aqueous solutions by a chelation mechanism. Response surface methodology (RSM) was used to optimize adsorption efficiency of nickel ions on Cs/PEO nanofibers. The combined effects of adsorption operating parameters, namely, the adsorbent dose, initial nickel ions concentration, temperature, and NaCl concentration, on adsorption efficiency were investigated using a central composite face-centered (CCF) design. Results showed that an optimal adsorption capacity of 64.4% was obtained under the following conditions: 75 mg of adsorbent dose, initial nickel concentration of 100 ppm, a temperature of 75 degrees C, and a 1M NaCl concentration.