Tailoring order in hierarchical structures is a key goal of bioinspired nanocomposite design. Recently, nacre-like materials have been developed by solvent evaporation methods that are scalable and attain advanced functionalities. However, understanding the alignment mechanisms of 2D-fillers, nanosheets or platelets, remains challenging. This work explores the possible pathways for nanocomposite ordering via orientation distribution functions. We demonstrate how the immobilization of 2D-materials via a (pseudo)-ne…