Poly(vinyl) butyral (PVB) nanofibers (NFs) and carbon nanotube (CNT) reinforced PVB NF composites were developed by using the Forcespinning (R) technology. PVB was dissolved in a mixture of ethanol and methanol (7:3 wt/wt) at various concentrations, and the solutions were spun at rotational speeds varying between 3,000 and 9,000 rpm. The CNT/PVB solutions were prepared using the same solvent ratio with varying the concentration of CNTs. The results show that the diameter of the PVB fibers increased with increasing rotational speed; however the standard deviation of the fiber diameter distribution decreased. The morphology and thermal properties of the developed fiber systems were studied by DSC, TGA, Raman, and FTIR. The effect of CNT on the mechanical properties of the developed fibers was investigated by carrying out tensile tests at different strain rates. Raman and FTIR analyses indicate a noncovalent - stacking interactions and hydrogen bonding between CNT and the PVB NFs. Adding CNT to the PVB NF matrix resulted in improved tensile strength by 150%. POLYM. ENG. SCI., 55:81-87, 2015. (c) 2014 Society of Plastics Engineers