“…Processing conditions can dramatically influence the obtained hierarchical structure. Several processes have been reported, such as suspension casting, doctor blading, vacuum-assisted self-assembly, melt compounding, in situ polymerization, etc. , About a decade ago, bioinspired polymer nanocomposites saw much advance with water-based and large-scale methodologies, akin to paper-making. ,,, Since then, the focus has shifted to the optimization of polymeric core–shell particles, followed by solvent removal. ,, The ideal conditions to realize aligned assemblies have been extensively adjusted. Nevertheless, these often are formed by intercalated structures, with restacking still observed at higher filler concentrations. ,− Above all, these efforts have led to a great number of mechanisms being proposed for polymer-particle association and (re)organization.…”