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Life systems are complex systems, and the self-assembly behaviour represents the transition from disorder to order and serves as a concrete indicator and starting point for understanding complex systems. Super-self-assembly behaviour was observed in the decoctions of various natural herbs, and this behaviour was characterized by multistep and multilevel assembly processes. The super-self-assemblies were multilevel particles resulting from inorganic–organic assembly, specifically observed as composite spheres, cubes, and tetragonal bipyramids. The preparation process was environmentally friendly and safe, and the resulting super-self-assemblies were regular in shape and rich in variety; this process has numerous possibilities for development and application in medicine and materials research.
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