In this study, a magnetic/polyetherimide-acrylonitrile composite nanofiber membrane with effective adsorption of nickel ions in an aqueous solution was created using a simple electrospinning method. Iron oxide nanoparticles (NPs) were stirred and ultrasonically dispersed into a polyetherimide-acrylonitrile solution to create a homogenous NPs suspension, which was placed in an electrospinning machine to produce a uniform and smooth nanofiber composite membrane. Nanoparticle incorporation into this membrane was confirmed using scanning electron microscope, energy dispersive X-ray spectroscopy (EDX), Fourier-transform infrared spectroscopy (FTIR), X-ray diffraction (XRD), and NPs aqueous stability from a leaching test. The high adsorption capability of the membrane on nickel ions was attributed to the combination of magnetic NPs, polyetherimide-acrylonitrile matrix, and the nanostructure of the membrane. A membrane containing magnetic NPs demonstrated the maximum adsorption capabilities (102 mg/g) of nickel ions in an aqueous solution. Various kinetic and isotherm models were applied to understand the adsorption behavior, such as pseudo-second-order kinetic and Langmuir isotherm models. A polyetherimide-acrylonitrile composite nanofiber membrane containing magnetic NPs could be used as an environmentally friendly and nontoxic adsorbent for the removal of nickel ions in an aqueous medium due to its ease of preparation and use and stability in aqueous mediums.