Hexagonal patterns of gold nanorods were made by assembling gold nanorod-coated poly(N-isopropyl acrylamide)microgels. The required population of nanorods on the microgels was achieved by attaching nanoparticle seeds onthe latter and growing them to nanorods. The various materials prepared were characterized by UV−vis spectroscopyand transmission electron microscopy. Similar experiments with nanoparticle-coated or prefabricated nanorod-coatedmicrogels did not give such hexagonal patterns. We suggest that the interlocking of nanorods leads to these regularstructures. This is the first report of a solution phase method for assembling nanorods into a hexagonal pattern.