Derived from Bombyx mori cocoons, regenerated silk fibroin (RSF) exhibits excellent biocompatibility, high toughness, and tailorable biodegradability. Additionally, RSF materials are flexible, optically clear, easily patterned with nanoscale features, and may be doped with a variety bioactive species. This unique combination of properties has led to increased interest in the use of RSF in sustainable and biocompatible electronic devices. In order to explore the applicability of this biopolymer to the development of future bioelectronics, the dielectric breakdown strength (E-bd) of RSF thin films was quantified as a function of protein conformation. The application of processing conditions that increased beta-sheet content (as determined by FTIR analysis) and produced films in the silk II structure resulted in RSF materials with improved E-bd with values reaching up to 400 V/mu m.