The hypothesis that novel material properties can be realized by blending polypeptides of starkly different amino acid composition has been tested. The polymer feedstock consisted of a novel recombinant elastin-like peptide (ELP) or a mixture of an ELP and a synthetic polypeptide, co-poly((L)-glutamic acid(4), (L)-tyrosine(1)) (PLEY), dissolved in water. Suitability of the polymers for materials fabrication has been assayed by electrospinning. Polymer structure in cast films and electrospun fibers by infrared (IR) spectroscopy. Scanning electron microscopy (SEM) analysis has revealed unique morphological properties of fibers spun from polymer blends of ELP and PLEY, properties not displayed by either polymer alone. Fluorescence microscopy showed that little if any phase separation occurred in the blended fibers. The materials of this research may present advantages for electrospun fiber applications in drug delivery and other areas. More generally, the present results will advance the growing field of peptide-based materials. (C) 2014 Elsevier Ltd. All rights reserved.