To improve the mechanical properties of zein films, a commercial white zein was reacted in glacial acetic acid (HAc) with glutaraldehyde (GDA) from 0.5 to 16% by weight based on the weight of zein. Amounts of 4% or higher GDA-modified zein, when cured in a closed system, generated a gel. That gel was insoluble in organic solvents known to solubilize zein. Zein solutions cast within a silicon rubber gasket sealed onto Teflon-coated plates, when air dried, generated 0.7-0.9-mm thick films. Those films from 8% GDA-modified zein had a water vapor permeability of 5.9 x 10(-8) g cm/Pa s m(2). Overall, results indicate that our thicker films gave higher water vapor permeability than values reported in the literature. To achieve consistent and comparable results with differential scanning calorimetry (DSC) and dynamic mechanical analyses (DMA), film samples had to be heated to remove residual HAc. An increase in the glass transition temperatures for those films from GDA-modification of zein, observed with both DSC and DMA, was attributed to the crosslinking of zein. Physical testing of tensile bars cut from GDA-modified zein films showed minor enhancement of tensile strength, percent elongation, and Young's modulus in the 0.5% GDA-modified zein films, which increased and leveled off with 4% or higher amounts of GDA for the modifications. When the 4 to 16% GDA results are averaged, the tensile strength for the modified zein films increased 1.8-fold when compared with unmodified zein control films. On the same note, percent elongation showed a 1.8-fold increase and Young's modulus showed a 1.5-fold increase. GDA reaction with zein generated films with improved tensile strength, ductility, and stiffness when compared with respective zein control films that retained their integrity when subjected to either boiling water or extensive soaking. (C) 2007 Wiley Periodicals, Inc.