“…To achieve higher strength beyond the record, covalent or ionic bonds, which are up to 10 times stronger than van der Waals interactions, − should be introduced in the internal structure of a CNTY. These advances can be realized by the chemical cross-linking of the CNT surface through the infiltrated binding materials, such as polymer or small organic molecule, thereby preventing pullout failures. − Nevertheless, the performance of the resulting materials has been disappointing ,,− because of inefficient cross-linking from a lack of understanding of the assembled CNTY structure and its load-bearing systems. Recently, the unique hierarchical structure of CNTY has been highlighted, and interbundle sliding was pointed out as the main hurdle to the fabrication of high-performance CNTY rather than intertubular slippage. ,, Therefore, CNTs inside the bundles can be assumed to be bound by intrabundle interactions, which are ideally composed of CNT stabilization energy and van der Waals interactions.…”