jats:titleAbstract</jats:title>jats:pSelf‐assembly is a very effective and popular method to create monolayers or thin films of aligned nanorods and ellipsoids. Nevertheless, there has been little attention to forming thick films of aligned nanorods using this approach. Here, the self‐assembly mechanism of nanorods coated with reduced graphene oxide in thick films with both a surface and a bulk alignment process is underpinned. The alignment method is robust and results in films with up to 50% higher volumetric density compared to nonaligned films of the same material. To optimize the coating process, an image processing script is implemented that quantifies the quality of the alignment based on a fast Fourier transform of nanorod electron microscope images. Based on this analysis, parameters are identified that influence the alignment to optimize the process for obtaining large area domains. Finally, dip‐coating, blade casting and zone coating are tested and compared and lithographically patterned substrates are used to template the self‐assembly process.</jats:p>