Alignment of layered double hydroxide platelets

► LDH tactoids were synthesized in stable and flocculating suspensions. ► Highly ordered planar random structures were made by filtration. ► In flocculating systems, edge-face interactions are overcome during filtration. ► Exfoliated LDH suspensions also assembled as rippled layered structures. ► These assemblies prepare for large-scale assembly of nacre-like nanocomposites.