This study focused on using chitosan (CS) as the functional polymer in the cellulose acetate (CA) matrix to provide reactive ion exchange sites for heavy metal ions. Pure CA and CA/CS blends (wt % 95:5, 90:10 and 85:15) were electrospun to determine the most qualified blend for the adsorption experiment. The morphologies of the electrospun nanostructured membranes were investigated using Scanning Electron Microscopy. The average fiber diameter was found to decrease with increasing CS concentration. CA and CS interaction was confirmed using Fourier Transform Infrared Spectroscopy. Upon characterization, the blend with 15% CS had the best properties for the adsorption process. The adsorption capacities of pure CA and CA/CS blend at different membrane loading and initial concentration showed a significant increase from 67.25 mg Cd2+/g pure CA membrane to 110.48 mg/g CS doped membrane. The experiment revealed that the adsorption kinetics of pure CA and CA/CS blend for Cd2+ were described by the pseudo-second order reaction model. The adsorption isotherm data for Cd2+on the surface of pure CA and CA/CS blend best fit the Freundlich isotherm and can be used to describe adsorption of Cd2+. This study produced an innovative nanostructured membrane for the removal of Cd2+ in wastewater.