Self-Healing in Cellulose-Based Materials: From Fundamentals to Future Perspectives

Self-healing materials have attracted increasing attention as a strategy to enhance durability, extend service life, and reduce maintenance in advanced material systems. Among these, cellulose-based self-healing materials represent a sophisticated intersection between sustainable macromolecular chemistry and adaptive materials science. This review provides a synthesis of recent advancements in the field, systematically categorizing materials derived from cellulose raw materials. We evaluate the fundamental chemical strategies employed to achieve autonomous repair, distinguishing between extrinsic mechanisms-utilizing cellulose-based micro/nano-capsules to sequester healing agents-and intrinsic mechanisms governed by dynamic covalent chemistry (Schiff-base, boronic ester, Diels-Alder) and supramolecular interactions (hydrogen bonding, metal-ligand coordination, and host-guest assemblies). The analysis highlights how cellulose's hierarchical structure and abundant surface functionality are leveraged to overcome the traditional trade-off between mechanical toughness and healing efficiency. Particular emphasis is placed on the transition from simple structural hydrogels to sophisticated multifunctional systems. These include ultra-stretchable strain and pressure sensors for e-skin applications, biocompatible and injectable matrices for chronic wound management and stem cell delivery, and advanced anti-freezing eutectogels for performance in extreme environments. Furthermore, we explore the integration of cellulose into traditional sectors, such as self-healing concrete utilizing microbe-induced calcification and smart, eco-friendly coatings for corrosion protection. Finally, we discuss critical challenges, including environmental stability, scalability, and the development of standardized evaluation protocols, providing a roadmap for the next generation of bio-derived, sustainable and intelligent materials.