Though the history of self‐healing materials stretches far back to the mid‐20th century, it is only in recent years where such unique classes of materials have begun to find use in bioelectronics—itself a burgeoning area of research. Inspired by the natural ability of biological tissue to self‐repair, self‐healing materials play a multifaceted role in the context of soft, wireless bioelectronic systems, in that they can not only serve as a protective outer shell or substrate for the internal electronic circuitry—analogous to the mechanical barrier that skin provides for the human body—but also, and most importantly, act as an active sensing safeguard against mechanical damage to preserve device functionality and enhance overall durability. This perspective presents the historical overview, general design principles, recent developments, and future outlook of self‐healing materials for bioelectronic devices, which integrates topics in many research disciplines—from materials science and chemistry to electronics and bioengineering—together.