This article reviews several classes of compliant materials that can be utilized to fabricate electronic muscles and skins. Different classes of materials range from compliant conductors, semiconductors, to dielectrics, all of which play a vital and cohesive role in the development of next generation electronics. This paper covers recent advances in the development of new materials, as well as the engineering of well characterized materials for the repurposing in applications of flexible and stretchable electronics. In addition to compliant materials, this article further discusses the use of these materials for integrated systems to develop soft sensors and actuators. These new materials and new devices pave the way for a new generation of electronics that will change the way we see and interact with our devices for decades to come.