Heterogeneous Functional Core-Shell Capsules Enabled by Nanoscale Spatial Assembly

Core-shell capsules provide an effective platform for storing active compounds and enabling on-demand delivery of programmed functions, serving as central components in the development of responsive polymers, drug carriers, and chemical absorbents. Complex capsules, composed of dense shells, liquid cores, and functional nanoparticles, are particularly appealing because their compositional heterogeneity offers tunable configuration and responsiveness. In this work, we present an approach to engineer site-specific functions in core-shell capsules. This method leverages organic ligands and inorganic corrugations to decorate nanoscale assemblies, allowing for precise control over their spatial distribution. We demonstrate that surface camouflage, whether soft or rigid, regulates the Pickering effect, thereby selectively directing nanofeatures to form shell-embedded or core-dispersed architectures. Further modulation of surface structure density enables nanoparticles to exclusively deposit on either the exterior or interior of the shell membrane. The generalizable mechanism is validated by the spatial arrangement of diverse nanoparticles with distinct compositions, shapes, and dimensions. The simultaneous yet respective deployment of various nanostructures endows core-shell capsules with heterogeneous functionalities, opening avenues for the creation of materials with sophisticated adaptability.