Patterned Binary Assembly of Polymer‐Grafted Gold Nanoparticles at Liquid‐Air Interfaces

Abstract Interfacial self‐assembly of polymer‐grafted nanoparticles (PGNPs) is a convenient approach for fabricating 2D nanocomposites. Co‐assembly of binary PGNPs at the liquid‐air interface offers opportunities to prepare 2D nanocomposites with structural diversity and tailored functions. However, it remains a great challenge for precisely controlling the interfacial co‐assembly structures of binary PGNPs. In this study, the interfacial assembly behavior of binary PGNPs is systematically investigated by varying the NP core and the polymer ligand. 2D nano‐discs with tunable segregation structures can be obtained by adjusting the size of the NP core and the length of the polymer ligand. The results demonstrated that the differences in the interfacial mobility and interfacial affinity of PGNPs dominated the structural diversity of the interfacial co‐assembly of binary PGNPs. This work advances the interfacial co‐assembly technology of PGNPs, marking a pivotal step toward its development as a refined and reliable micro‐nano fabrication methodology.