Biosensor technology is a fast-growing area in biomedicine as the demand for rapid analysis is increasing nowadays. A significant problem that biosensors face is the degradability and failure of biosensor materials, mainly due to temperature, pH, or the state of applied stress. Innovative material design and synthesis methods are required to close the reusability gap for these devices. Moreover, new materials are needed to ensure a better and cheaper diagnosis, especially in countries where diagnostic equipment is not readily available. Self-healing materials, a novel class of smart materials, can repair themselves without external stimuli when damage occurs to the structure. Deformations can be self-healed, giving rise to multiple applications in biotechnology when constant diagnosis monitoring is needed. These materials are ideal for various applications, including flexible electronics and biosensors. This review summarizes the synthesis methods, properties, and applications of self-healing materials in biosensors. Furthermore, emphasis is given to the sustainability and environmental aspects of these materials.