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In line with the scientific community effort to create efficient and accessible ways to remove arsenic from water, this work shows the ability of immobilized magnetic iron oxide nanoparticles (MIONs) into electrospun poly(vinyl alcohol) (PVA) membranes to adsorb As(V) from water. Electrospinning solutions were prepared using two different approaches: suspending dry MIONs in a PVA solution and in situ synthesis of the MIONs. Results show a high adsorption capacity of 68 mg/g and well dispersed particles in the nanofibers. These straightforward and scalable methods are promising alternatives for water remediation.