The ability to repair damage spontaneously, which is termed self-healing, is an important survival feature in nature because it increases the lifetime of most living creatures. This feature is highly desirable for rechargeable batteries because the lifetime of high-capacity electrodes, such as silicon anodes, is shortened by mechanical fractures generated during the cycling process. Here, inspired by nature, we apply self-healing chemistry to silicon microparticle (SiMP) anodes to overcome their short cycle-life. We show that anodes made from low-cost SiMPs (~3–8 µm), for which stable deep galvanostatic cycling was previously impossible, can now have an excellent cycle life when coated with a self-healing polymer. We attain a cycle life ten times longer than state-of-art anodes made from SiMPs and still retain a high capacity (up to ~3,000 mA h g−1). Cracks and damage in the coating during cycling can be healed spontaneously by the randomly branched hydrogen-bonding polymer used.