Summary Effects of hydration on silk fibroin film material properties were investigated for water-annealed and MeOH treated samples. After hydration, thickness increased 60% for MeOH immersed films, while water-annealed samples remained constant. TGA determined MeOH immersed films had an 80% mass loss due to water, while water-annealed had a 40% mass loss. O2 permeability was greater in MeOH immersed films with Dk values of 10 (10−11·mLO2·cm)/(cm·s·mmHg), while water-annealed films had Dk values of 2 (10−11·mLO2·cm)/(cm·s·mmHg). All films showed a decrease in Young’s modulus and increased plastic deformation by two orders of magnitude when submerged in saline solution. FTIR revealed water-annealed films increased in β-sheet content with increasing water vapor, while MeOH immersed films did not change.

The functional properties of six distinct electrospun silk material groups were evaluated to assess conformational and biocompatible characteristics related to wound dressings. In a hydrated state, all six silk matrices exhibited absorption, water vapor transmission, oxygen permeation and enzymatic biodegradation suitable for full-thickness wound sites. Employing constrained drying techniques, silk concentration was a determinate factor influencing material structural properties related to the storage and distribution of such wound dressing systems. Subsequently, three electrospun silk models demonstrated ideal biomaterial properties with potential utility for wound dressings.

Front Cover: Constrain‐dried electrospun silk materials exhibit flat pliable membrane conformations and demonstrate a potential utility to provide an impermeable barrier to bacterial pathogens, manage wound site edema, and support time‐synchronized tissue regeneration biotherapies as a resorbable full‐thickness wound dressing. Further details can be found in the article by S. E. Wharram, X. Zhang, D. L. Kaplan, and S. P. McCarthy* .

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