To investigate the effects of co-solvents on the morphology of nano-scale zein materials, zein solutions were electrospun with different co-solvent ratios of EtOH/H2O. Different zein solution concentrations were used to study the effects of the zein content on the electrospun materials. The resulting electrospun materials were all characterized using field-emission scanning electron microscopy (FE-SEM) and transmission electron microscopy (TEM). The diameters of the electrospun nanoparticles and nanofibers were found to increase when increasing the EtOH ratio at certain zein concentrations. Furthermore, increasing the zein content changed the morphology of the electrospun materials from nanoparticles to nanofibers.