Abstract: Methods are provided for making layer-by-layer assemblies that comprise axial geometry nanoparticles. Such methods include forming a first layer on a substrate that comprises an axial nanoparticle, forming a second layer on the substrate that comprises an axial nanoparticle, where the first and second layers are aligned to respective first and second orientations. The disclosure also provides for multilayer materials having a first layer including a first polyelectrolyte and a first axial geometry nanoparticle which is substantially aligned along a first orientation. The multilayer material also includes a second layer including a second polyelectrolyte and a second axial geometry nanoparticle species having axial geometry, where the second nanoparticle species is substantially aligned along a second orientation which is distinct from the first orientation.