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.