nanostructures can be organized into a hierarchical architecture, thus giving their excellent physical and chemical properties. [1,6,7] Accordingly, protein-based biomimetic mineralization has been became an inspiration for synthesis of the highperformance organic-inorganic hybrid materials. Recently, many reviews have been published to report the progress of biomimetic organic-inorganic nanocomposites. Wang et al. reviewed the preparation of layered organic-inorganic nanocomposites inspired by nacre and indicated the advantages and disadvantages of various biomimetic strategies. [8] Zhang et al. summarized recent research on graphene-based artificial nacre nanocomposites and focused on the interface interactions design. [9] Wang et al. discussed functional protein-based organic-inorganic hybrid nanomaterials with an emphasis on the novel preparation methods, resulting nanostructures, and their potential applications in drug delivery and enzymatic catalysis. [10] Yao et al. summarized the fabrication of artificial layered structural nanocomposites based on the different inorganic building blocks, such as clays, ceramic nanoparticles, layered double hydroxides, calcium carbonate, and graphene. [11] Zhao et al. overviewed the synthesis and performance enhancement strategies for different dimensional nacre-inspired materials such as 1D fibers, 2D films, and 3D bulk composites. [6] The reviews mentioned above are mainly focused on the strategies to construct layered organic-inorganic hybrid materials and their applications in various fields, and the interface design to obtain high-performance structural nanocomposites. Although it has been demonstrated that the protein components function as templates involving in the biomineralization, the regulation on their structure and the mediation of proteins on the fabrication of hybrid materials are seldom presented, mainly because of their complex molecular structure and uncontrollable selfassembly process in vitro. Amyloid is a kind of insoluble self-assembly peptide or protein aggregate displaying polymorphic mesoscopic structures. [12] Even though the amyloids are originally discovered as the pathological hallmarks of human neurodegenerative diseases, it is found that there are also many nonpathogenic functional amyloid aggregates implicated in biological processes occurring in a variety of organisms ranging from simple bacteria to humans, such as the adhesive property of E. coil biofilms, [13] biosynthesis Protein assembly with ordered architecture plays an important role in the formation of natural organic-inorganic hybrid materials, and also determines their distinguished mechanical, optical, and biochemical properties. Nevertheless, it has been a huge challenge to synthesize materials with hierarchical structure accurately mimicking the natural hybrid materials in vitro. In the past decade, protein amyloid aggregates, due to their diverse and controllable nanostructures and unique properties, have been developed as superior templates or building blocks to fabricate f...