Abstract Wereport a simple approach for the direct and nondestructive assembly ofmulti-sheeted single-walled carbon nanotube book-like macrostructures(buckybooks) with good control of the nanotube diameter, the sheetpacking density, and the book thickness during the floating catalyticgrowth process. The promise of such buckybooks is highlighted bydemonstrating their high capacitance and high-efficiency molecularseparation by directly using them as a binder-free electrode and as afilter, respectively. Our approach also provides a flexible andreliable way to easily assemble various other types of nanotubes intobook-like or even more sophisticated sandwich-like hybridmacrostructures, realizing the shape-engineering of one-dimensionalnanostructures to macroscopic well-defined architectures for variousapplications.