Nanoparticle assembly and colloidal processing are two techniques with the goal to fabricate materials and devices from preformed particles. While colloidal processing has become an integral part of ceramic processing, nanoparticle assembly is still mainly limited to academic interests. It typically starts with the precise synthesis of building blocks, which are generally not only considerably smaller than those used for colloidal processing, but also better defined in terms of size, shape, and size distribution. Their arrangement into 1D, 2D, and 3D architectures is performed with great accuracy well beyond what is achieved by colloidal processing. At the same time, the final assembly is not sintered such that the intrinsic, nanospecific properties of the initial building blocks are preserved or even lead to collective behavior. However, in contrast to colloidal processing the structures accessible by nanoparticle assembly are often limited to a small length scale. The review presents selected examples of nanoparticle assembly and colloidal processing with the goal to reveal the capabilities of these two techniques to fabricate novel materials from preformed building blocks, and also to demonstrate the immense opportunities that would arise if the two methods could be combined with each other.