Abstract
<jats:p>Multi-walled carbon nanotubes (MWCNTs) have potential for a range of industrial applications. However, their utility is constrained by challenges related to processing and dispersibility due to their tendency to aggregate in solvents, especially polar ones. This study describes the use of a metal-organic cage (MOC) to non-covalently functionalize and disperse MWCNTs in both water and polar organic solvents. The MOC interacts with the CNTs through stacking interactions, displaying a clear preference for thinner tubes. An understanding of the functionalization of the CNTs was obtained through calorimetric, microscopic and spectroscopic techniques. The counterion-responsive solubility behavior of the MOCs provided a means to transport CNTs between liquid phases. The resulting MOC-bound CNTs exhibit improved dispersibility, enhancing their processability while preserving the intrinsic properties associated with the sp2 carbon framework. Importantly, the cages can be removed, allowing the material to revert to its pristine state. This work thus introduces a reversible, non-covalent strategy for CNT functionalization based on coordination cages, offering a route to CNT processing within and across liquid phases.</jats:p>