Bioinspired Bifunctional MOF Synergizing Superhydrophobicity‐Photothermal Adsorption via Narrow‐Bandgap Engineering for On‐Demand Oil Remediation

Abstract The design of dual‐mode remediation platforms using flexible metal–organic frameworks (MOFs) to synergize superhydrophobicity and broadband photothermal activity remains a fundamental challenge for programmable solar‐driven oil/water separation in spill remediation. A cactus‐inspired nanoneedle‐architected CuTCNQ MOF (TCNQ = tetracyanoquinodimethane) is developed through bandgap engineering and self‐assembly, synergizing intrinsic superhydrophobicity with a narrow bandgap ( E g = 0.36 eV). The passive CuTCNQ@CM membrane achieves gravity‐driven oil/water separation (99.53 ± 0.29% efficiency, 84.22 ± 3.82 kL·m −2 ·h −1 flux), retaining 98.26% performance after 20 cyclic separation tests, where ultralong 1D nanostructures amplify surface roughness and capillary forces through synergistic wettability enhancement and separation kinetics optimization. In parallel, the active CuTCNQ@PU system exhibits 98.96% broadband solar absorption (200–2500 nm) and a high solar‐thermal conversion efficiency (STCE) of 93.64%, rapidly heating to 90.6 °C under 1‐sun irradiation to reduce crude oil viscosity by 98.93%, enabling ultrafast adsorption (84.1 ± 2.3 g·g −1 capacity, 436.7 ± 23.5 g·g −1 ·min −1 rate). The design pioneers dual‐mode superhydrophobicity‐bandgap MOFs by unifying passive/active functionalities through nanostructuring. The scalable synthesis, combined with sunlight‐triggered adsorption, delivers an uninterrupted remediation platform–passively treating bulk spills and actively addressing viscous residues via light‐controlled synergy, advancing energy‐efficient environmental technologies.