The development of polymers that can spontaneously repair themselves after mechanical damage would significantly improve the safety, lifetime, energy efficiency and environmental impact of man-made materials. Most approaches to self-healing materials require the input of external energy, healing agents, solvent or plasticizer. Despite intense research in this area, the synthesis of a stiff material with intrinsic self-healing ability remains a key challenge. Here, we show a design of multiphase supramolecular thermoplastic elastomers that combine high modulus and toughness with spontaneous healing capability. The designed hydrogen-bonding brush polymers self-assemble into a hard-soft microphase-separated system, combining the enhanced stiffness and toughness of nanocomposites with the self-healing capability of dynamic supramolecular assemblies. In contrast to previous self-healing polymers, this new system spontaneously self-heals as a single-component solid material at ambient conditions, without the need for any external stimulus, healing agent, plasticizer or solvent.