Gold nanorods (AuNRs) have attracted significant attention over the past several decades for a variety of applications and there has been steady progress with regards to their synthesis and modification. Despite these advances, the assembly of AuNRs into well‐organized hierarchical assemblies remains a formidable challenge. Specifically, there is a need for tools that can fabricate assemblies of nanorods over large length scales at low cost with the potential for high‐throughput manufacturing. Langmuir‐Blodgettry is a monolayer deposition technique which has been primarily applied to amphiphilic molecules, but which has recently shown promise for the ordering of functionalized nanoparticles residing at the air‐water interface. In this work, Langmuir‐Blodgett deposition is explored for the formation of AuNR arrays for enhanced surface‐enhanced Raman spectroscopy (SERS) sensing. In particular, both surface modification of the AuNRs as well as subphase modification with cysteamine were evaluated for AuNR array fabrication.