Nanofibers formed by electrospinning provide very large surface areas which can enhance material performance in filtration and product separation. In this work, we explore atomic layer deposition (ALD) as a means to coat and protect electrospun nylon-6 nanofibers. Exposing nylon to trimethyl aluminum (TMA) during ALD of aluminum oxide results in significant fiber degradation. Protecting fibers with a bilayer of ALD ZnO and an organic-inorganic hybrid polymer by molecular layer deposition maintains the shape of the original nanofibers, but chemical modification is still detected. These coating processes may help enable nanofibers with stable physical properties under chemical exposure. (C) 2011 The Electrochemical Society. [DOI: 10.1149/1.3609046] All rights reserved.