Summary: A micrometer rod morphology was produced by self‐assembly of poly(oxypropylene)amine (POP‐amine) modified montmorillonite. The requisite primary structure was prepared by intercalation of the layered clay with POP‐amine salts. During the drying process, the primary units self‐assemble into micro‐rods that are 100–800 nm wide and 2–40 μm long. The stacking process may involve two complimentary forces – the POP hydrophobic effect and the silicate ionic interaction – acting in separate directions.