Bioinspired Ultrasmall‐Bandgap MOF‐Integrated Superhydrophobic Textiles via In Situ Self‐Assembly: Enabling Next‐Generation Multifunctional Smart Textiles

Abstract The integration of bio‐inspired nanostructured metal‐organic frameworks (MOFs) with textiles opens new frontiers for smart wearable systems. This study develops a mechanically robust superhydrophobic AgTCNQ‐MOF hybrid fabric via in situ self‐assembly, mimicking cactus spines to achieve water contact and sliding angles of 159.2° and 1.8°, respectively. The optimized textile demonstrates multifaceted functionality: 1) Ultrahigh oil‐water separation performance (efficiency: 98.4%; flux: 18.0 kL·m −2 ·h −1 ); 2) Anti‐icing capacity extending freezing onset from 105 s to 685 s under −20 °C; 3) Full‐spectrum UV resistance (UVA: 2.5%, UVB: 2.7%) with 99.8% antimicrobial efficacy; 4) Autonomous self‐cleaning via contaminant‐removing rolling droplets; and 5) Outstanding mechanical flexibility (6000 cycles) coupled with ultrahigh solar‐thermal efficiency (91.5%) enabled by AgTCNQ‐derived ultrasmall‐bandgap (0.47 eV) engineering, a notable advancement over conventional systems. A covalent interfacial anchoring strategy ensures exceptional durability, maintaining superhydrophobicity after 30 abrasion cycles or 200 h UV exposure. The ultrasmall‐bandgap of AgTCNQ uniquely optimizes photon‐to‐thermal conversion while maintaining multifunctionality, which is a key innovation differentiating this platform. This synergy between bandgap‐engineered nanoporosity and textile flexibility enables real‐time environmental responsiveness. Such integration bridges nanotechnology and textile engineering to address wearable‐environmental challenges, advancing applications in medical wearables, industrial filtration, and adaptive robotics.