Because of its biomimetic similarity with extracellular matrix, electrospinning has potential in tissue engineering applications. Electrospun polymer mats form non-woven, three-dimensional, inter-connective, nanofibrillar networks. Mechanical property characterization of nanofibers is still in its early stages. Crosslinkers, such as glutaraldehyde (GA), are added to nanofibers post-processing to improve mechanical properties of the electrospun fiber mats. GA is widely available and easily forms iminic bonds with biopolymers through a Schiff-base reaction. Natural polymers are preferred over synthetic polymers in biomedical engineering, but the mechanical integrity of natural polymers needs to be improved. Chitosan, the N-deacetylated derivative of chitin, is found in crustacean and arthropod shells, and also in fungi and yeast. Basic in nature, chitosan has applications in wound healing and tissue repair, antimicrobial resistance, metal ion adsorption, and cell adhesion. Chitosan consists of acetyl-glucosamine and glucosamine units with �-1-4 glycosidic linkages. Poly-ethylene oxide (PEO) is a biocompatible, non-toxic, inert polymer that can bond with chitosan to improve the charge-carrying capacity and viscosity of electrospinning blends. In this study, a chitosan and PEO blend were electrospun and vapor crosslinked with GA for various time periods to determine whether the tensile and compressive mechanical integrities of the nanofibers could be improved with increasing exposure to vapor crosslinking. Nanoindentation, uniaxial tensile tests, solubility, FT-IR, and SEM characterization analyses were used to confirm these trends. The mechanical studies confirmed that the structural properties of the crosslinked nanofibers improved. GA vapor crosslinking improved stiffness and decreased ductility of the electrospun mats. In the solubility studies, increased exposure time to crosslinking led to improved structural integrity, surface color clarity, and resistance to dissolution. In the FT-IR studies, the intensity of the imine bond (1620-1660 cm-1) increased as crosslinking time increased. SEM fiber counts verified that exposure to GA vapor crosslinking increased the average fiber diameter.