Engineering Carbon Nanotube‐Based Photoactive COF to Synergistically Arm a Multifunctional Antibacterial Hydrogel

Abstract Enhancing the covalent organic framework (COF)’s photocatalytic ability synergistically with gelling formulations remains an urgent challenge for extended bio‐applications. Herein, COF is homogeneously coated on an oxidized carbon nanotube (OCNT) and coordinated by Fe 3+ to obtain tubular nanocomplex OCNT@COF‐Fe (O@CF). The results showed that the photodynamic reactive oxygen species (ROS) generation ability of O@CF is enhanced due to the wrapped OCNT and the coordinated Fe 3+ , which can respectively serve as intermolecular charge transfer channel and electron acceptors/substrates (O 2 and H 2 O) adsorbent to narrow the energy band gaps, increase the light absorption, and decrease the photogenerated carrier recombination. Synergistically, O@CF exhibited pH‐dependent peroxidase and catalase activities, which further enhanced ROS generation and relieved hypoxia, respectively. Meanwhile, O@CF possessed degradation of COF coatings‐dependent photothermal performances. Then, O@CF is evenly incorporated into Schiff base hydrogel via the COF coating‐participated covalent cross‐linking, to obtain an electroconductive hydrogel OCNT@COF‐Fe@Gel (O@CF@G). This O@CF@G can not only improve the mechanical properties of pure gel but also inherit the multifunction of O@CF. Consequently, it can well adhere to diabetic wounds for imbibition, drug‐resistant biofilm elimination, gram‐positive and negative bacteria killing, hypoxia alleviation, and intercellular electrical signal conduction, thus accelerating wound healing.