Droplet evaporation is a simple method to induce organization of Au nanorods into ordered superstructures. In general, the self-assembly process occurs by evaporation of aqueous suspensions under strictly controlled experimental conditions. Here we present formation of large area ordered vertical arrays by droplet evaporation of Au nanorod organic suspensions. The uncontrolled (free air) evaporation of such suspensions yielded to formation of ordered nanorod domains covering the entire area of a 5 mm diameter droplet. Detailed investigation of the process revealed that nanorods organized into highly ordered vertical domains at the interface between solvent and air on a fast time scale (minutes). The self-assembly process mainly depended on the initial concentration of nanorod solution and required minimal control of other experimental parameters. Nanorod arrays displayed distinct optical properties which were analyzed by optical imaging and spectroscopy and compared to results obtained from theoretical calculations. The potential use of synthesized arrays as surface-enhanced Raman scattering probes was demonstrated with the model molecule 4-aminobenzenthiol.