Mechanical characterization of nanofiber mats is an underexplored area in biomaterial engineering. In this study, a chitosan-poly(ethylene oxide) copolymer blend was electrospun and crosslinked with glutaraldehyde (GA) for various time periods. The tensile and compressive mechanical integrity of the nanofibers was analyzed with increasing exposure to vapor crosslinking. Solubility, scanning electron microscopy characterization, Fourier transform infrared, uniaxial tensile tests, and nanoindentation analyses were used to identify these trends. The mechanical studies confirmed that the GA vapor crosslinking increased the stiffness and decreased the ductility of the electrospun mats. Increased exposure time to crosslinking led to changes in the mat surface color and resistance to dissolution. Scanning electron microscopy fiber counts verified that exposure to GA vapor crosslinking increased the average fiber diameter. By the use of vapor phase deposition, mechanical properties continued to change throughout the study. The crosslinking exposure time could be chosen to accommodate in vivo mechanical loading. (C) 2008 Wiley Periodicals, Inc.