Precise organization of matter across multiple length scales is of particular interest because of its great potential with advanced functions and properties. Here we demonstrate a simple yet versatile strategy that enables the organization of hydrophobic nanoparticles within the covalent organic framework (COF) in an emulsion droplet. The interfacial polymerization takes place upon the addition of Lewis acid in the aqueous phase, which allows the formation of COF after a crystallization process. Meanwhile, the interaction between nanoparticles and COF is realized by the use of amine-aldehyde reactions in the nearest loci of the nanoparticles. Importantly, the competition between the nanoparticle self-assembly and interfacial polymerization allows control over the spatial distribution of nanoparticles within COF. As a general strategy, a wide variety of COF-wrapped nanoparticle assemblies can be synthesized and these hybridized nanomaterials could find applications in optoelectronics, heterogeneous catalysis and energy chemistry.

跨多个长度尺度的物质的精确组织特别令人感兴趣，因为它具有先进的功能和特性，具有巨大的潜力。在这里，我们演示了一种简单而通用的策略，该策略能够在乳液液滴的共价有机框架（COF）中组织疏水​​性纳米颗粒。在水相中添加路易斯酸时发生界面聚合，这允许在结晶过程之后形成COF。同时，通过在纳米颗粒的最接近位点使用胺-醛反应来实现纳米颗粒与COF之间的相互作用。重要的是，纳米粒子自组装和界面聚合之间的竞争允许控制纳米粒子在COF中的空间分布。作为一般策略，