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Producing densely packed arrays of nanoscopic anisotropic objects, while necessary for applications in photovoltaic and field emission devices, presents considerable challenges. Here, we present findings on the phase separation of ligand-functionalized nanorods in a polymer matrix under an applied electric field. Densely packed hexagonal arrays of nanorods are produced by this method, where the rods are oriented in the direction of the applied field. Minimization of interfacial energy between the array of nanorods and the surrounding polymer serves to corral the nanorods into the densely packed arrays observed. These findings carry implications toward advancing organic−inorganic heterojunction photovoltaic devices that are expected to benefit from the oriented, densely packed ordered arrays of nanorods produced here.