High-performance polymer electrolyte membranes (PEMs) with excellent proton conductivity, gas barrier property, and membrane stability are desired for future fuel cells. Here we report the development of PEMs based on our proposed new concept "Nanofiber Framework (NfF)." The NfF composite membranes composed of phytic acid-doped polybenzimidazole nanofibers (PBINf) and Nafion matrix show higher proton conductivity than the recast-Nafion membrane without nanofibers. A series of analyses reveal the formation of three-dimensional network nanostructures to conduct protons and water effectively through acid-condensed layers at the interface of PBINf and Nafion matrix. In addition, the NfF composite membrane achieves high gas barrier property and distinguished membrane stability. The fuel cell performance by the NfF composite membrane, which enables ultra-thin membranes with their thickness less than 5 gm, is superior to that by the recast-Nafion membrane, especially at low relative humidity. Such NfF-based high-performance PEM will be accomplished not only by the Nafion matrix used in this study but also by other polymer electrolyte matrices for future PEFCs. (C) 2016 Elsevier B.V. All rights reserved.