“…In the past few years, many research groups have reported on assembly techniques of micrometer-sized mesocrystals of platinum, magnetite, lead sulfide, and silver, among other materials. ,− They have shown remarkable structures of mesocrystals, which are perfectly regular and feature well-defined facets, like “classical” crystals. Commonly, nanocrystals are assembled into mesocrystals either via “drying mediated assembly methods” or via the “gas phase diffusion technique”. ,,,, Often, the structure of these assemblies is characterized incompletely, with the main emphasis on the study of explicit properties or specific applications of mesocrystals. ,,, Nevertheless, investigations with a combination of small- and wide-angle X-ray scattering techniques (SAXS and WAXS) as well as advanced microscopy techniques allow a full structural analysis of self-assembled superstructures based on nanoparticles of different compositions and shapes. ,,,,,, The recently developed angular X-ray cross-correlation analysis (AXCCA) method allows the determination of the superlattice distortion and relative orientation of nanoparticles in mesocrystals with high precision. − Similarly, great effort is put on how these crystals nucleate and grow and how the kinetics influence the nonclassical crystallization of mesocrystals. ,,− Furthermore, there are many interesting results on how growth conditions can impact the final structure of mesocrystalline films. − Accordingly, different superlattice structures can be obtained by solvent evaporation from dispersions with different dispersion agents as well as from nanoparticles stabilized by different ligands. , However, an understanding of the morphogenesis of macroscopic mesocrystals is still essentially lacking. Specifically, the exact parameters which influence the crystal structure and morphology, including packing arrangement and orientational order, remain largely unexplored.…”