Taking inspiration from natural materials, composite materials can be reinforced by creating matrix architectures that can better accommodate and control internal stresses. Despite the recent success in the synthesis of artificial assemblies for local reinforcement through the introduction of oriented fibers and plates into host multilayered composites, there is a lack of fundamental understanding of the factors that determine mechanical properties. Moreover, designing building blocks and interfaces that facilitate higher resistance and energy dissipation is highly challenging. When the intrinsic material is fixed, the mechanical and tribological properties can be further adjusted. In this study, europium oxide nanosheets are arranged in interlocked-junction superstructures that resist sliding at junction points, thereby enhancing the mechanical properties of the nanosheet assemblies compared to those of the conventional face-to-face superstructures formed by parallel nanosheets. Furthermore, the crystalline origin of building blocks is revealed by demonstrating that faulty crystal nanosheets adopting an amorphous structure are different from single-crystal nanosheets, with the former exhibiting superior mechanical reinforcement and improved abrasive resistance.