Nanoscale fibers with embedded, aligned, and percolated non‐functionalized multiwalled carbon nanotubes (MWCNTs) were fabricated through electrospinning dispersions based on melt‐compounded thermoplastic polyurethane/MWCNT nanocomposite, with up to 10 wt.‐% MWCNTs. Transmission electron microscopy indicated that the nanotubes were highly oriented and percolated throughout the fibers, even at high MWCNT concentrations. The coupling of efficient melt compounding with electrospinning eliminated the need for intensive surface functionalization or sonication of the MWCNTs, and the high aspect ratio as well as the electrical and mechanical properties of the nanotubes were retained. This method provides a more efficient technique to generate one‐dimensional nanofibers with aligned MWCNTs.
