Pure and doped ZnO nanofibers with Al and Mg were successfully synthesized via an electrospinning method using a sol gel containing Polyvinylpyrrolidone as a spinning aid and a zinc nitrate precursor. Calcination of the doped and undoped electrospun nanofibers was conducted at 500 degrees C in air, and the resultant structures were analyzed by X-ray diffraction (XRD) and Raman spectroscopy. The diameter of the doped nanofibers decreased with increasing viscosity and conductivity, as measured by scanning electron microscopy (SEM) and transmission electron microscopy (TEM). Energy dispersive spectroscopy (EDS) showed that Mg and Al are present in ZnO nanofibers. The pressure composition isotherm (PCI) demonstrated that the capacity of hydrogen storage in pure zinc oxide nanofibers is a factor of two greater than that of zinc oxide nanoparticles. However, Al-doped ZnO nanofibers have the highest capacity of hydrogen storage (2.81 wt%) at room temperature. Copyright (C) 2012, Hydrogen Energy Publications, LLC. Published by Elsevier Ltd. All rights reserved.