In article number 2007346, Dae-Hyeong Kim, Taeghwan Hyeon, Donghee Son, and co-workers develop a durable and fatigue-resistant soft bidirectional neuroprosthetic device composed of a biocompatible nanocomposite of gold-nanoshell-coated silver flakes dispersed in a tough, stretchable, and self-healing polymer. The electrical conductivity of our neuroprosthetics spontaneously recovers even after repetitive degradations by irregular and severe mechanical deformations.