The present invention provides for compositions, methods and devices for rapidly converting silk fibroin solution into a silk fibroin gel using direct application of voltage, in a process called electrogelation. The silk fibroin gel may be reversibly converted back to liquid form by applying reverse voltage or may be converted further to ²-sheet structure by applying shear force or other treatments. The electrogelated silk may be used as an extracted bulk gel, spray or stream of gel for processing into materials or devices, or may be used as silk gel coating to devices. Active agents may be embedded in the silk gel for a variety of medical applications. The electrogelated silk exists as a piezoelectric silk material comprising a mixture of silk fibroin proteins having silk I conformation and silk ²-sheet structure. Silk electrogelation process of the present invention is useful in variety of applications such as tissue engineering, medical device or implants, drug delivery, soft robotics or motion associated technology.
