Surfactant‐mediated co‐existence of single‐walled carbon nanotube networks and cellulose nanocrystal mesophases

Hybrids comprising cellulose nanocrystals (CNCs) and percolated networks of singlewalled carbon nanotubes (SWNTs) may serve for the casting of hybrid materials with improved optical, mechanical, electrical, and thermal properties. However, CNC‐dispersed SWNTs are depleted from the chiral nematic (N*) phase and enrich the isotropic phase. Herein, we report that SWNTs dispersed by non‐ionic surfactant or triblock copolymers are incorporated within the surfactant‐mediated CNC mesophases. Small‐angle X‐ray measurements indicate that the nanostructure of the hybrid phases is only slightly modified by the presence of the surfactants, and the chiral nature of the N* phase is preserved. Cryo‐TEM and Raman spectroscopy show that SWNTs networks with typical mesh size from hundreds of nanometers to microns are distributed equally between the two phases. We suggest that the adsorption of the surfactants or polymers mediates the interfacial interaction between the CNCs and SWNTs, enhancing the formation of co‐existing mesostructures in the hybrid phases.