Since the Lycurgus Cup was made in the 4th century, metal nanoparticles have attracted much interest due to the characteristics of the plasmonic and metamaterials that show beautiful colors. Despite these fascinating properties, the practical use is limited because it is difficult to control the orientation of the plasmonic nanoparticles. Here, highly aligned plasmonic gold nanorods are obtained using self-assembled DNA material. Simple mechanical shearing results in long-range DNA-gold nanorod arrays which show parallel, perpendicular, and zigzag configurations due to the competition between the shear force and DNA elasticity. The resulting surface plasmonic resonance properties of the aligned DNA-gold nanorods film show highly polarization-dependent behavior in a large area, which is critical for optical and photonic applications. This simple way to form anisotropic plasmonic films can be used for plasmonic nanoparticles in potential applications such as displays and sensors.The ORCID identification number(s) for the author(s) of this article can be found under https://doi.org/10.1002/adfm.201703790.Recently, a few methods for controlling the GNRs based on the liquid crystal (LC) material used as a host medium were suggested to control the guest material-GNRs with external stimuli such as electric field, [21] magnetic field, [22] and mechanical force, [9] in which GNRs are spontaneously arranged with the LC director [9,21,[23][24][25] or trapped in the defect of LCs. [26] Among the various types of host LC materials, it is well known that lyotropic LC (LLC) is the most promising candidate for controlling GNRs because LLC itself is dispersed in the solvent, making it easy to homogeneously mix with GNR. Indeed, the phase transition occurs as a function of the solute concentration, here LLC material and GNR, meaning that various conformations of GNR can be achieved. LLC is found in condensed biomaterials such as DNA, [27,28] food dyes, [29] cellulose, [30,31] collagen, [32,33] and bacteriophage, [34,35] which are abundantly produced every year. Among these LLC materials, DNA extracted from plant or fish are easy to get and indeed very cheap compared with typical synthetic polymers and LC materials used in the practical applications. Particularly, DNA can be used as a building block to make small structures since DNA has the specific sequences that can be spontaneously assembled together to make the programmable structure such as origami. [36,37] Here, we fabricate well-oriented GNRs in DNA medium. Compared with other LLC, the orientation of DNA is easily controlled by applying simple mechanical shearing [38][39][40] (Table S1, Supporting Information). Thus, the DNA was selected as the medium to orient GNRs. The DNA material used in this study is salmon sperm DNA duplex (purchased from Sigma-Aldrich, St. Louis, MO, USA) with a Gaussian distribution in base pairs, for which the center point is ≈2000 base pairs and the corresponding length is ≈680 nm. [41] The DNA material in aqueous solution forms the LLC phase at t...