Using polarized Raman spectroscopy, we have recorded Raman spectra from individual electrospun Nylon-6 nanofibers. Analysis of these single-fiber spectra, compared to those of unoriented and oriented Nylon-6 films, indicates significant molecular orientation. Because electrospinning produces fibers in a jet with a large strain rate, this molecular orientation is expected. We present quantitative measurements of molecular orientation in a single nanofiber and compare these to those of film samples. Such measurements could yield information about the uniformity of the electrospinning process and resulting fibers, and may also allow comparison between spectrally measured orientation functions and single-fiber mechanical properties. (c) 2008 Elsevier Ltd. All rights reserved.