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The co‐assembly of spherical colloids and surfactant–cyclodextrin microtubes yields a library of dynamic colloid‐in‐tube structures, including helices. In situ observations of these structures, including their thermo‐reversible assembly and disassembly, demonstrate the potential of the interplay between molecular and colloidal self‐assembly, thereby providing a novel route to temperature‐sensitive particle alignment and release. [ABSTRACT FROM AUTHOR]

Anisotropic and binary colloids self-assemble into a variety of novel supracolloidal structures within the thermo-switchable confinement of molecular microtubes, achieving structuring at multiple length scales and dimensionalities. The multistage self-assembly strategy involving hard colloidal particles and a soft supramolecular template is generic for colloids with different geometries and materials as well as their binary mixtures. The colloidal architectures can be controlled by colloid shape, size, and concentration. Colloidal cubes align in chains with face-to-face arrangement, whereas rod-like colloids predominantly self-organize in end-to-end configurations with their long axis parallel with the long axis of the microtubes. The 1D microconfinement imposed on binary mixtures of anisotropic and isotropic colloids further increases the diversity of colloid-in-tube structures. In cube-sphere mixtures, cubes may act as additional confiners, locking in colloidal sphere chains, while a 'colloidal Morse code' is generated where rods and spheres alternate in the case of rod-sphere mixtures. The versatile confined colloidal superstructures including their thermoresponsive assembly and disassembly are relevant for the development of stimulus-responsive materials where controlled release and encapsulation are desired. [ABSTRACT FROM AUTHOR]

Hierarchical self‐assembly is often exploited by nature to build complex functional entities. A similar approach yielded a library of dynamic colloid‐in‐tube structures, such as colloidal zigzags, double‐ and triple‐helices, by utilizing the thermo‐reversible co‐assembly of colloidal spheres and molecular microtubes, as reported by J. Huang, A. V. Petukhov, et al. in their Communication on page 3364 ff. The assembly and disassembly of these structures near human body temperature was explored in situ and in real time. [ABSTRACT FROM AUTHOR]

Hierarchical, bottom‐up, self‐organization processes of nano‐ and microscale building blocks constitute an important design route for stimulus‐responsive materials. On page 313, Andrei V. Petukhov and co‐workers demonstrate that a rich variety of novel supracolloidal structures emerge from the self‐organization of various shape‐anisotropic colloids and binary mixtures of isotropic and anisotropic colloids in 1D microconfinement. [ABSTRACT FROM AUTHOR]