Nature offers inspiration for the development of high-performance synthetic materials. Extensive studies on the universal adhesion and self-healing behavior of mussel byssus reveal that a series of reversible molecular interactions occurring in byssal plaques and threads play an essential role, and the mussel-inspired chemistry can serve as a versatile platform for the design of self-healing materials. In this Perspective, we provide an overview of the recent progress in the detection, quantification, and utilization of mussel-inspired reversible molecular interactions, which includes the elucidation of their binding mechanisms via force-measuring techniques and the development of self-healing materials based on these dynamic interactions. Both conventional catechol-medicated interactions and newly discovered chemistry beyond the catechol groups are discussed, providing insights into the design strategies of advanced self-healing materials via mussel-inspired chemistry.