As information technologies move from electron- to photon-based systems, the need to rapidly modulate light is of paramount importance. Here, we study the evolution of the electric-field-induced alignment of gold nanorods suspended in organic solvents. The experiments were performed using an all-fiber optofluidic device, which enables convenient interaction of light, electric fields, and the nanorod suspension. We demonstrate microsecond nanorod switching times, three orders of magnitude faster than a traditional Freederickcz-based liquid crystal alignment mechanism. We find that the dynamics of the alignment agrees well with the Einstein–Smoluchowski relationship, allowing for the determination of the rotational diffusion coefficient and polarizability anisotropy of the nanorods as well as the effective length of the ligands capping the nanorods. The ability to dynamically control the optical properties of these plasmonic suspensions coupled with the point-to-point delivery of light from the fiber component, as demonstrated in this work, may enable novel ultrafast optical switches, filters, displays, and spatial light modulators.