Electronically interfacing with the nervous system for the purposes of health diagnostics and therapy, sports performance monitoring, or device control has been a subject of intense academic and industrial research for decades. This trend has only increased in recent years, with numerous high-profile research initiatives and commercial endeavors. An important research theme has emerged as a result, which is the incorporation of semiconducting polymers in various devices that communicate with the nervous system─from wearable brain-monitoring caps to penetrating implantable microelectrodes. This has been driven by the potential of this broad class of materials to improve the electrical and mechanical properties of the tissue-device interface, along with possibilities for increased biocompatibility. In this review we first begin with a tutorial on neural interfacing, by reviewing the basics of nervous system function, device physics, and neuroelectrophysiological techniques and their demands, and finally we give a brief perspective on how material improvements can address current deficiencies in this system. The second part is a detailed review of past work on semiconducting polymers, covering electrical properties, structure, synthesis, and processing.