In this paper, the PVA/HNTs composite nanofibers with well-enhanced mechanical properties were successfully prepared by electrospinning technique. The structure and properties of the composite nanofibers were characterized by TEM, XRD, FT-IR, and DSC. The results indicated that the highly oriented and dispersed HNTs wrapped in polymer matrix were achieved by inducing function during electrospinning processing. The mechanical properties of the PVA/HNTs composite nanofibers depended on HNTs content were investigated, which showed 72.4% increase in tensile strength at optimal filling content. Copyright (c) 2016 John Wiley & Sons, Ltd.