Single cellulose nanocrystal rod-templated right-handed imine-linked covalent organic frameworks for enantioselective recognition.

Chiral materials from cellulose nanocrystals (CNCs) usually derive from left-handed helical organization formed by collective self-assembly, while the direct transfer of the intrinsic right-handed chirality of individual CNC nanorods into well-defined hybrid architectures remains largely unexplored. Elucidating this chirality transfer process is essential for understanding the multihierarchical chirality transcription of cellulose. Herein, we present an interfacially confined Schiff-base polymerization that uses single right-handed CNC rods as chiral templates to fabricate core-shell CNC@covalent organic framework (COF) hybrids. Electrostatic enrichment of protonated amine monomers and subsequent acid-catalyzed confined condensation at the CNC-water interface directs the oriented growth of an imine-linked COF shell, effectively transcribing the single-rod chirality into a supramolecular helical organization with amplified chiroptical activity. The resulting hybrid retains the right-handed chiroptical response derived from the CNC template and exhibits a significantly enhanced Cotton effect, achieving a g abs of -6.23 × 10-3. Moreover, the chiral confined porous microenvironment enables enantioselective adsorption of ofloxacin, affording capacities of 8.22 mg g-1 for S-ofloxacin and 3.03 mg g-1 for R-ofloxacin, whereas the corresponding pristine COF is nearly nonselective. This work establishes a strategy for transforming intrinsic nanoscale chirality into functional hybrid materials and provides a platform for designing chiral porous materials for recognition, separation, and advanced photonic applications.