Compression‐Triggered Instantaneous Nanoplastic Release From Dynamic Hydrogen‐Bonded LDH@Cellulose Semi‐Flexible Micro‐Nano Aerogel for Sustainable Water Remediation

ABSTRACT Nanoplastic (NPs) pollution represents one of the most persistent environmental crises of our time, requiring breakthrough material technologies for effective remediation. In this study, we engineer a semi‐flexible micro‐nano structured N‐modified cellulose nanofibers@layered double hydroxide (N‐CNF@LDH) composite aerogel through a dynamic hydrogen bonding and coordination interactions to achieve efficient removal of NPs, in which the LDH nanoflower clusters are uniformly anchored on the nitrogen‐modified cellulose honeycomb skeleton. Under the action of dynamic hydrogen bonds, the structure undergoes spontaneous reorganization at new equilibrium positions upon release of external force, leading to a reversible opening‐closing motion within the floral clusters. This design enables ultrahigh NPs adsorption (3648 mg·g −1 ) through reversible inter‐petal channel opening, while compression‐triggered petal contraction achieves instantaneous release (96% within only 10 s), exhibiting a desorption kinetics rate nearly three orders of magnitude higher than conventional adsorbents. Besides, the dynamic network enables rapid structural reconstruction of N‐CNF@LDH through H‐bond assembly, maintaining 80.4% NPs capacity and 95.2% shape recovery after 100 cycles. Exhibiting outstanding NPs removal performance in various real‐world water systems while remaining cost‐effective, this material breaks through the fundamental capacity‐regeneration compromise in environmental remediation.