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  1. Abstract

    Planar nanocrystal/bulk heterostructures are transformed into 3D architectures by taking advantage of the different chemical and mechanical properties of nanocrystal and bulk thin films. Nanocrystal/bulk heterostructures are fabricated via bottom‐up assembly and top‐down fabrication. The nanocrystals are capped by long ligands introduced in their synthesis, and therefore their surfaces are chemically addressable, and their assemblies are mechanically “soft,” in contrast to the bulk films. Chemical modification of the nanocrystal surface, exchanging the long ligands for more compact chemistries, triggers large volume shrinkage of the nanocrystal layer and drives bending of the nanocrystal/bulk heterostructures. Exploiting the differential chemo‐mechanical properties of nanocrystal and bulk materials, the scalable fabrication of designed 3D, cell‐sized nanocrystal/bulk superstructures is demonstrated, which possess unique functions derived from nanocrystal building blocks.

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