Supramolecular Engineered Naphthalenediimide/Aramid Nanofiber Dressings for NIR Photothermal Repair and Regeneration of Infected Conjunctival Defects

Damage to the conjunctiva, a critical ocular‐surface barrier, readily leads to secondary infection, exacerbated inflammation, and delayed re‐epithelialization. Near‐infrared (NIR) photothermal therapy (PTT) provides a remote, non‐antibiotic approach for conjunctival repair, but the delicate ocular surface requires low‐power irradiation and thus highly efficient photothermal dressings. Here, we report Et 2 DPNDI·2I, a NIR‐responsive naphthalenediimide (NDI)‐derived pyridinium salt. Single‐crystal analysis reveals compact cation‐anion packing reinforced by C‐H···I, C‐H···O, and I···π interactions, which broadens NIR absorption and promotes nonradiative decay, enabling a photothermal conversion efficiency (PCE) of 81.6% under 808 nm irradiation. Incorporating Et 2 DPNDI·2I into aramid nanofiber (ANF) networks affords conformal, mechanically robust NDI/ANF composite films. Hydrogen bonding, π–π interactions, and electrostatic interactions between the NDI pyridinium salt and ANFs preserve high photothermal performance, giving a maximum film PCE of 67.8%. These films demonstrate good cytocompatibility and effective photothermal antibacterial activity against E. coli and S. aureus . In a rabbit model of bacteria‐infected bulbar conjunctival defects, NDI/ANF‐20, with a maximum PCE of 61.1%, achieves the best balance between infection control and tissue regeneration. Multi‐omics analyses and experimental validation further associate this outcome with reduced inflammation, improved mitochondrial function, and restored lipid homeostasis. Overall, this work presents a supramolecular‐engineering strategy for constructing high‐performance NDI/ANF dressings for NIR photothermal repair and regeneration of infected conjunctival defects.