Self-Healing Polymer Nanocomposites: Mechanisms, Structure–Property Relationships, and Emerging Applications

Self-healing polymer nanocomposites are increasingly investigated as damage-tolerant materials for structural and functional applications; however, their engineering translation remains limited by the difficulty of achieving high mechanical reinforcement while retaining sufficient polymer mobility for effective repair. Previous reviews have largely summarized healing chemistries or nanofiller classes but have rarely established quantitative structure–property–healing relationships or resolved contradictory trends reported across studies. In this review, we develop an integrated framework that links polymer network architecture, nanofiller geometry/percolation behavior, and interfacial dynamics to healing kinetics, and we compile quantitative design windows for nanofiller loading, percolation thresholds, activation conditions, and durability metrics. The synthesis reveals that healing performance is maximized within intermediate filler contents near the percolation regime, whereas excessive nanofiller loading commonly suppresses healing by nanoscale confinement and interphase immobilization despite improving modulus and conductivity. Finally, we propose application-oriented design rules and benchmarking priorities, emphasizing standardized fracture/fatigue-based evaluation, multi-cycle healing retention, and scalable interphase engineering as the key pathways for translating self-healing nanocomposites from laboratory demonstrations to validated engineering systems.