The bottom-up construction of Frank–Kasper (FK) phases in soft matter requires intricating tuning to balance entropic and enthalpic interactions. In contrast, sophisticated rules have been established in Metallurgy to dictate the packing structures of metal alloys. Inspired by alloy metallurgy, we develop a new self-sorting approach to construct nanostructures in condensed soft matters. This approach utilizes blends of nano-sized giant molecules to construct supramolecular motifs (“mesoatoms”) with controlled size heterogeneity, which is the key in rational design of diverse FK nanostructures. Especially, the scarcely observed thermodynamically stable Laves C14 and C15 phases are widely found. This approach sheds light on next-generation material engineering which allows nanostructure construction in a more predictable and straightforward way

软物质中Frank-Kasper（FK）相的自下而上构造需要复杂的调整以平衡熵和焓相互作用。相反，在冶金学中已经建立了复杂的规则来规定金属合金的堆积结构。受合金冶金学的启发，我们开发了一种新的自分选方法来构造凝聚态软物质中的纳米结构。这种方法利用纳米级巨分子的共混物来构建具有受控大小异质性的超分子基序（“中原子”），这是合理设计各种FK纳米结构的关键。尤其是，广泛发现了几乎没有观察到的热力学稳定的Laves C14和C15相。这种方法为下一代材料工程提供了启示，该技术允许以更可预测和更直接的方式构造纳米结构