To integrate the exceptional properties of nanoscale building blocks into macroscopic devices, manufacturing methods that achieve control of nanoparticle (NP) assembly up to macroscale dimensions have to be developed. [1][2][3][4][5][6][7][8] In this regard, structural hierarchy emerges as a powerful strategy for creating functional materials, involving a precise control of composition and shape across several length scales. [1,[9][10][11][12][13] NPs can be assembled into larger structures by exploiting and further controlling their inherent intermolecular and surface forces. [3,14] Thus, by taking advantage of the short-range forces, colloidal self-assembly appears as a successful bottom-up approach for the development of new materials and their further integration into novel devices. Moreover, by specifically designing the nanobuilding blocks, the macroscopic behavior of the resulting engineered materials can be

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3D printing is used to self‐assemble surface‐functionalized nanoparticles into supercrystalline macrostructures. The obtained columns feature high strength, favorably comparing to hierarchical composite materials, known for their exceptional mechanical properties. Further details can be found in the article, number http://doi.wiley.com/10.1002/adem.202000352, by A. John Hart, Gerold A. Schneider and co‐workers.