“…The assembly of nano building blocks into three-dimensional hierarchical architectures is enormously appealing from the perspectives of both fundamental research and practical applications due to the sophisticated assembly process and the extraordinary properties of the resultant materials. , As powerful sources of inspiration, natural organisms possessing the advantages of multilevel hierarchy, morphological diversity, and large length scale have been extensively pursued for hierarchical architecture assembly. − However, despite tremendous progress, mimicking the intrinsic features of natural structural hierarchy through nanostructure assembly is still challenging. , In particular, the natural hierarchical organisms are generated through growth evolution, which can adapt to their growth environments, allowing the formation of entities with diversified shapes across a wide length scale. , In contrast, artificially assembled hierarchical materials are normally restricted to regular shapes (such as rods and spheres) and specific sizes . This is primarily attributed to the inherent requirements of traditional assembly, that is, straightforward assembly of nanostructures for the thermodynamic equilibrium of the system, which confines the morphology of the resulting assemblage to a regular shape and specific size to achieve minimum surface energy. − Hence, to address this issue, it is imperative to explore a novel strategy distinct from traditional assembly to create hierarchical materials with greater diversity in terms of 3D shapes and dimensions.…”