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Granular materials, composed of densely packed particles, are known to possess unique mechanical properties that are highly dependent on the surface structure of the particles. A microscopic understanding of the structure‐property relationship in these systems remains unclear. Here, supra‐nanoparticle clusters (SNPCs) with precise structures are developed as model systems to elucidate the unexpected elastic behaviors. SNPCs are prepared by coordination‐driven assembly of polyhedral oligomeric silsesquioxane (POSS) with metal‐organic polyhedron (MOP). Due to the disparity in sizes, the POSS‐MOP assemblies, like their classic nanoparticles counterparts, ordering is suppressed, and the POSS‐MOP mixtures will vitrify or jam as a function of decreasing temperature. An unexpected elasticity is observed for the SNPC assemblies with a high modulus that is maintained at temperatures far beyond the glass transition temperature. From studies on the dynamics of the hierarchical structures of SNPCs and molecular dynamic simulation, the elasticity has its origins in the interpenetration of POSS‐ended arms. The physical molecular interpenetration and inter‐locking phenomenon favors the convenient solution or pressing processing of the novel cluster‐based elastomers.

The intrinsic conflicts between mechanical performances and processability are main challenges to develop cost‐effective impact‐resistant materials from polymers and their composites. Herein, polyhedral oligomeric silsesquioxanes (POSSs) are integrated as side chains to the polymer backbones. The one‐dimension (1D) rigid topology imposes strong space confinements to realize synergistic interactions among POSS units, reinforcing the correlations among polymer chains. The afforded composites demonstrate unprecedented mechanical properties with ultra‐stretchability, high rate‐dependent strength, superior impact‐resistant capacity as well as feasible processability/recoverability. The hierarchical structures of the hybrid polymers enable the co‐existence of multiple dynamic relaxations that are responsible for fast energy dissipation and high mechanical strengths. The effective synergistic correlation strategy paves a new pathway for the design of advanced cluster‐based materials.

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Three novel amphiphilic BODIPY derivatives were prepared and their photophysical properties in THF/water mixtures with varying fractions of water were investigated. BDP-1 could self-assemble into different vesicle architectures in aqueous solution, while BDP-2 and BDP-3 with more hydrophilic abilities formed spherical and worm-like micelles. The BODIPY derivatives could be absorbed by HeLa cells and showed no apparent toxicity during the course of the test. In particular, unlike traditional amines or morpholinyl functionalized lysosome fluorescent probes, BDP-1 nanovesicles without targeted groups exhibit red emission and show effective lysosome biological imaging. Co-staining experiments with lysosome specific trackers further confirmed the disassembly of BDP-1 nanovesicles in lysosomes. This research provides a new avenue of using probes without targeting the structural unit to stain special organelles and shows potential applications in cell imaging fields.

A novel water-soluble supramolecular dendronized polymer (SDP) was prepared through cucurbit[8]uril (CB[8])-naphthalene host−guest interaction. The composition ratio between BDP and CB[8] of as-prepared luminescent supramolecular polymer was confirmed by 1 H NMR technique and mass spectrometry. In addition, atomic force microscopy (AFM) images showing the polymer chain length up to 150 nm and height up to 1.75 nm unambiguously demonstrate the supramolecular polymer formation. This work might be useful for designing other main chain supramolecular dendronized polymers.

Films that can maintain their flexibilities and conductivities under low humidity and broad temperature range represent the next generation of solid-state proton conductors, which would extend the applications of energy storage and conversion devices in extreme environments. Owing to their strong interactions with poly­(ethylene oxide) (PEO), polyoxometalates (POMs), a group of nanoscale metal oxide clusters, can form stable nanocomposites with PEO and fully inhibit its crystallization, facilitating the fast dynamics of PEO chains/segments, as evidenced from dielectric spectroscopy studies. It thus enables the fast proton transportation in the PEO matrix and the improvement of the composites’ proton conductivities. With POMs’ loading ratio approaching to 70% wt, the nanocomposite’s proton conductivity reaches as high as 6.86 × 10–3 S cm–1 at 100 °C in anhydrous environment. The composites’ mechanical properties can be further optimized upon the tuning of PEOs’ molecular weight and finally, a flexible, self-supported anhydrous proton conductor can be obtained, which also demonstrates high compatibility to electrodes. The nanocomposite can maintain promising proton conductivities ranging from −20 to 100 °C in an anhydrous environment, enabling the fabrication of long-term robust performance of supercapacitor devices under extreme conditions, which has never been achieved before.