Architecting Durability: Synergies in Assembly, Self-Repair, and Advanced Characterization of Carbon Nanotube Materials

Carbon nanotubes (CNTs) have remarkable mechanical, electrical, and thermal properties, making them highly attractive as foundational elements for advanced materials. However, translating their nanoscale potential into macroscale reliability and longevity requires a holistic design approach that integrates precise architectural control with robust damage mitigation strategies. This review presents a synergistic perspective on enhancing the durability of CNT-based systems by critically examining the interplay between molecular assembly, self-repair mechanisms, and the advanced characterization techniques required for their validation. We first establish how foundational architectural control—achieved through strategies like chemical functionalization, field-directed alignment, and dispersion—governs the ultimate performance of CNT materials. A significant focus is placed on advanced functionalization, such as fluorination, and its verification using high-powered spectroscopic tools, including X-ray photoelectron spectroscopy (XPS) and near-edge X-ray absorption fine structure (NEXAFS) spectroscopy. Subsequently, this manuscript delves into the mechanisms of self-repair, systematically analyzing both the intrinsic capacity of the carbon lattice to heal atomic-level defects and the extrinsic strategies that incorporate engineered healing agents into composites. This discussion is uniquely supplemented by an exploration of the experimental techniques, such as electron energy loss spectroscopy (EELS) and Auger electron spectroscopy (AES), that provide crucial evidence for irradiation-induced healing dynamics. Finally, we argue that a “characterization gap” has limited the field’s progress and highlight the critical role of techniques like in situ Raman spectroscopy for quantitatively monitoring healing efficiency at the molecular level. By identifying current challenges and future research frontiers, this review underscores that the creation of truly durable materials depends on an integrated understanding of how to build, repair, and precisely measure CNT-based systems.