“…Grzelczak et al realized binary self-assembly of gold nanowires with nanospheres and GNRs . Through modulating by using polymer brush coatings, DNA double helices, and metal–metal/π–π interactions, various freestanding GNRs assemblies can be well obtained. − Furthermore, these GNRs-based self-assembly systems, either assembly↔disassembly transformation or resulting assemblies, have been employed for the studies of sensing, detecting, imaging, catalyzing through the coupling effects of GNRs’ LSPR themselves or with LSPR and fluorescence/Raman scattering/circular dichroism. − However, just like any other NCs, for GNRs, while their self-assembly studies have obtained substantial achievements in the aspects of superstructure construction, property manipulation, and various application exploration; the self-assembly mechanism research cannot obviously keep up with the pace, ascribed to the lack of appropriately quantitative approaches for the corresponding study. It is rather difficult to demonstrate the precise chemical/supramolecular pictures at both the NCs’ surface and interbuilding blocks during self-assembly, except for a few limited systems (for example, DNA-functionalized building blocks self-assemble by Watson–Crick interactions). , …”