Noncovalent interactions can maintain the three-dimensional structures of biomacromolecules (e.g., polysaccharides and proteins) and control specific recognition in biological systems. Supramolecular chemistry was gradually developed as a result, and this led to design and application of self-healing materials. Self-healing materials have attracted attention in many fields, such as coatings, bionic materials, elastomers, and flexible electronic devices. Nevertheless, self-healing materials for biomedical applications have not been comprehensively summarized, even though many reports have been focused on specific areas. In this Review, we first introduce the different categories of supramolecular forces used in preparing self-healing materials and then describe biological applications developed in the last 5 years, including antibiofouling, smart drug/protein delivery, wound healing, electronic skin, cartilage lubrication protection, and tissue engineering scaffolds. Finally, the limitations of current biomedical applications are indicated, key design points are offered for new biological self-healing materials, and potential directions for biological applications are highlighted.