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Controlling the degradation process of silk is an important and interesting subject in biomaterials field. In the present study, silk fibroin films with different secondary conformations and nanostructures were used to study the degradation behavior. Silk fibroin films with highest β-sheet content achieved highest degradation rate, different from the previous studies. A new degradation mechanism revealed that degradation behavior of silk fibroin was related to not only crystal content, but also hydrophilic interaction and crystal-noncrystal alternant nanostructures. The hydrophilic blocks of silk were firstly degraded. Then, the hydrophobic crystal blocks which were formerly surrounded and immobilized by hudrophilic blocks, became free particles and moved into solution. Based on the mechanism, which enables the process more controllable and flexible, controlling the degradation behavior of silk fibroin without sacrificing other performances such as mechanical or hydrophilic properties become feasible, and this would greatly expand the applications of silk as a biomedical material.

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