or loop shapes. The particles (i.e., building blocks) could be spherical spheres, cubes, rods, disks, bipyramids, etc. Another type of NNs are formed when the particles are connected by linkers or threaded onto a string or stem (type II). The strings or stems could be polymer chains, nanowires, nanorods, nanotubes, nanobelts, etc. The third type of NNs is comprised of particles that are deposited on a robust support to form a periodic arrangement that resembles a necklace (type III). The supports could be polymers, nanorods, nanotubes, nanofibers, etc.Although these three types of necklacelike nanostructures are quite different from each other in shape and morphology, they all possess some common features, such as intrinsic high surface area, abundant transport channels, exposure of each component to the surface, and multiscale roughness of the surface (as compared to other 1D nanogeometries such as rods, wires, fibers, tubes, and belts). Most type I necklace-like nanostructures are discontinuous structures that consist of 1D aligned building blocks. The interparticle distance between the building blocks is crucial to the properties of the necklace-like nanostructures. When the interparticle distance is sufficiently short, coherent optical properties are obtained through near-field coupling of their surface plasmon resonances. [11] Additionally, electromagnetic coupling between isolated nanoparticles (NPs) is much lower than the electromagnetic interactions between NPs in close proximity in a necklace-like nanostructure. [12] The static electromagnetic interactions between neighboring metallic NPs in necklacelike nanostructures may contribute to an enhancement of nonlinear optical properties and surface-enhanced Raman scattering (SERS) effect. For type II necklace-like nanostructures, the bead-on-string architecture may provide facile electron transfer and percolation, an open scaffold for ion accessibility, maximized surface area to volume ratio, and good strain tolerance, all of which are highly conducive to energy storage. [13] For type III necklace-like nanostructures, the percolating clusters of metallic or semiconductor NPs show different electrical properties because of their interparticle electron transport. [14] Thus, decorating metallic or semiconductor NPs over a robust support to form necklace-like structures is a promising strategy to craft single-electron devices. [15] Notably, NNs possess a unique surface morphology that is distinctly different from the smooth surface of nanorods, nanotubes, and nanowires. Necklace-like structures possess multiscale roughness, which renders themThe shape-controlled synthesis of nanocrystals remains a hot research topic in nanotechnology. Particularly, the fabrication of 1D structures such as wires, rods, belts, and tubes has been an interesting and important subject within nanoscience in the last few decades. 1D necklace-like micro/nanostructures are a sophisticated geometry that has attracted increasing attention due to their anisotropic and periodic structure, in...