The remarkable mechanical, electrical, thermal and optical properties of carbon nanotubes (CNTs) are only valid for individual particles, and are generally lost when bulk CNT materials are integrated in devices.^[1-3] The controlled manufacturing of macroscopic functional and high-performance CNT-materials, retaining the compelling properties of individual tubes, has hence become of paramount importance to allow their full exploitation within commercial products.

Herein we report an unprecedented sequential engineering of the architecture of CNT materials, from the nano-, to the micro- and macroscale level. Specifically, we report on a a microfluidic assisted methodology to generate discrete 3D CNT microparticles, to be employed in large area self-assembly processes, enabling a high degree of hierarchization and tailoring of the CNT material.

Such controlled multiscale engineering, paves the way for the implementation of a property-conservative manufacturing of CNT-based materials, boosting their performance–to–cost ratio, and integration in a vast set of applications with high societal and industrial impact, such as high performance filters, catalysts, and energy storage devices.