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We report a simple approach for the direct and nondestructive assembly of multi-sheeted single-walled carbon nanotube book-like macrostructures (buckybooks) with good control of the nanotube diameter, the sheet packing density, and the book thickness during the floating catalytic growth process. The promise of such buckybooks is highlighted by demonstrating their high capacitance and high-efficiency molecular separation by directly using them as a binder-free electrode and as a filter, respectively. Our approach also provides a flexible and reliable way to easily assemble various other types of nanotubes into book-like or even more sophisticated sandwich-like hybrid macrostructures, realizing the shape-engineering of one-dimensional nanostructures to macroscopic well-defined architectures for various applications.

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