Highly ordered hierarchical biomolecule-inorganic structures, such as bone, dentine, eggshell, and marine mollusc shells, are ubiquitous in nature. [1] The artificial organization of nature-inspired, biomolecule-templated hierarchical inorganic materials is a key challenge in enabling many nanotechnological applications.[2] "Bottom-up" self-assembly is a widely applied strategy for synthesizing and fabricating ordered hierarchical/multilevel spatial structures or morphologies from components ranging from nanometers to micrometers in size. Alternatively, "top-down" lithographic approaches allow for arbitrary geometrical designs and superior nanometer-level precision, accuracy, and registration. Template-assisted self-assembly (TASA) combines bottom-up self-assembly with top-down patterned templates to eliminate defects and induce registration and orientation in thin-film materials, providing rich opportunities to produce biomimetic multilevel hierarchies. [3] Using TASA, the orientation and periodicity of zerodimensional (0D) spherical block copolymer microdomains, colloid crystals, and metal nanoparticles and 1D metal oxide nanotubes/nanowires were guided into 2D/3D hierarchical spatial architectures. [3a,d, 4] In these systems, the use of biomolecular building blocks has attracted great attention because of their biocompatibility, inherent molecular-recognition properties, and facile use in bottom-up fabrication. Recently, DNA origami-like triangles (with precise banding of gold nanocrystals) were successfully placed and oriented on lithographically patterned surfaces. [5] These systems are the most typical examples of selectively aligning 2D assemblies to date. The successful selective alignment, placement, and arrangement of anisotropic 2D/3D hierarchically mesostructured assemblies with sufficient long-range order, however, have rarely been reported. [6]