Non-close-packed (NCP) two-dimensional (2D) ordered nanoparticle (NP) arrays have attracted considerable attention due to their unique properties; however, their efficient and large-scale fabrication remains challenging. In this study, we present a facile yet effective point-to-point adsorption method for producing large-area NCP 2D ordered gold NP (AuNP) arrays using a rapidly assembled block copolymer (BCP) micelle monolayer as a template. By capitalizing on the inherent monodispersity and soft corona characteristics of BCP micelles, combined with the industrial compatibility of dip-coating technology, we achieved efficient and scalable fabrication of ordered BCP micelle monolayers. Key processing parameters, including dip-coating speed, micelle concentration on morphology of the templates, were systematically optimized. These micelle-monolayers serve as templates for the point-to-point adsorption of AuNPs, resulting in well-defined NCP 2D arrays. Adsorption mechanism was revealed to be an electrostatic interaction between protonated P4VP cores and size-matched AuNPs stabilized by citrate. The fabricated AuNP arrays demonstrate high performance in nano-floating-gate transistor memory devices, exhibiting a memory window of 54 V, on/off ratio of 3.8 × 10³, and endurance stability over 110 write-read-erase-read cycles. These performance metrics significantly surpass those of conventional BCP-only templates, which showing great promise for applications in optoelectronic devices.

A solvent annealing-induced structural reengineering approach is exploited to fabricate polymersomes from block copolymers that are hard to form vesicles through the traditional solution self-assembly route. More specifically, polystyrene-b-poly(4-vinyl pyridine) (PS-b-P4VP) particles with sphere-within-sphere structure (SS particles) are prepared by three-dimensional (3D) soft-confined assembly through emulsion-solvent evaporation, followed by 3D soft-confined solvent annealing upon the SS particles in aqueous dispersions for structural engineering. A water-miscible solvent (e.g., THF) is employed for annealing, which results in dramatic transitions of the assemblies, e.g., from SS particles to polymersomes. This approach works for PS-b-P4VP in a wide range of block ratios. Moreover, this method enables effective encapsulation/loading of cargoes such as fluorescent dyes and metal nanoparticles, which offers a new route to prepare polymersomes that could be applied for cargo release, diagnostic imaging, and nanoreactor, etc.