Advances in the field of nature-inspired/derived biomaterials have been revolutionizing the production of next-generation biomedical devices over the past few years, and will continue to make impacts in the field. Of special interest is the application of biodegradable materials in the fabrication of fully organic, intrinsically flexible, thin film devices. Components with precisely patterned micro- or nano-scale circuits can provide different functions as microelectrodes, biosensors, and supercapacitors. Advantages include the ability to provide conformal contact at non-planar biointerfaces, being able to be degraded at controllable rate, and invoking minimal reactions within the body. These factors present great potential as implantable devices for in-vivo applications, while also addressing concerns with “electronic waste” by being intrinsically degradable. The fabrication of such flexible bioelectronics requires a careful optimization of mechanical properties, electrical conductivity, and precise fabrication using materials that are often not easily adapted to such processes. One option of particular interest is the construction of biocompatible and biodegradable, flexible bioelectronics based on silk proteins. In this work, we present the combination of photo-crosslinkable silk proteins and conductive polymers to precisely fabricate flexible devices for the sensing of different targets of interest. A facile and scalable photolithography is applied to fabricate flexible substrates with conductive micropatterns which show tunable electrical and mechanical properties. Competitive conductivity, as well as excellent biocompatibility and controllable biodegradability are shown. Through this work, the possibility of making next-generation, fully organic, flexible bioelectronics is explored.