Tensile strength, Young’s modulus, and toughness of electrospun nylon 6 non-woven fiber mats were improved by increasing individual nanofiber strength and fiber–fiber load sharing. Single-walled carbon nanotubes (CNTs) were used as reinforcement to increase the strength of the electrospun nylon 6 nanofibers. Young’s modulus, tensile strength, and toughness of the nylon 6 non-woven fiber mats electrospun from 20 wt % solutions increased 51%, 87%, and 136%, respectively, after incorporating 1 wt % CNTs into the nylon 6 nanofibers. Three methods were investigated to enhance fiber–fiber load sharing: increasing friction between fibers, thermal bonding, and solvent bonding. The addition of beaded nylon 6 nanofibers into the non-woven fiber mats to increase fiber-fiber friction resulted in a statistically significantly increase in Young’s modulus over comparable smooth non-woven fiber mats. After annealing, tensile strength, elongation, and toughness of the nylon 6 non-woven fiber mats electrospun from 20 wt % + 10 wt % solutions increased 26%, 28%, and 68% compared to those from 20 wt % solutions. Solvent bonding with formic acid vapor at room temperature for 30 min caused increases of 56%, 67%, and 39% in the Young’s modulus, tensile strength, and toughness of non-woven fiber mats, respectively. The increases attributed to increased individual nanofiber strength and solvent bonding synergistically resulted in the improvement of Young’s modulus of the electrospun nylon 6 non-woven fiber mats.
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