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The stepwise self-assembly of hollow plasmonic vesicles with vesicular membranes containing strings of gold nanoparticles (NPs) is reported. The formation of chain vesicles can be controlled by tuning the density of the polymer ligands on the surface of the gold NPs. The strong absorption of the chain vesicles in the near-infrared (NIR) region leads to a much higher efficiency in photoacoustic (PA) imaging than for non-chain vesicles. The chain vesicles were further employed for the encapsulation of drugs and the NIR light triggered release of pay loads. This work not only offers a new platform for controlling the hierarchical self-assembly of NPs, but also demonstrates that the physical properties of the materials can be tailored by controlling the spatial arrangement of NPs within assemblies to achieve a better performance in biomedical applications. [ABSTRACT FROM AUTHOR]

The hierarchical assembly of multifunctional materials is challenging. In their Communication on page 15809 ff., Z. H. Nie, X. Y. Chen, and co‐workers report the stepwise assembly of block‐copolymer‐tethered gold nanoparticles into strings that subsequently fold into vesicles with chain‐like ordering of the nanoparticles in the membrane. The resulting vesicular assemblies can be used for photoacoustic imaging and drug delivery owing to their strong absorption in the near‐infrared region. [ABSTRACT FROM AUTHOR]