Hierarchically structured functional nanocomposites may exhibit new properties and are in demand to meet the growing material needs for advanced technology. To this end, it is imperative to simultaneously achieve structural control over multiple length scales and to develop rapid, scalable fabrication to limit degradation of nanoparticle properties due to exposure to processing environment and for compatibility with nanomanufacturing. We show that a wavelength dependent isotropic-to-anisotropic optical transition can be obtained by forming three-dimensional (3-D) ordered arrays of gold nanoparticles in thin films of supramolecular nanocomposites, highlighting the importance of structural control over the spatial arrangement of nanoparticles. By optimizing only the solvent fraction in the film during solvent annealing, hierarchically structured thin films of supramolecular nanocomposites can be produced in oneminute. The assembly kinetics are governed by the energetic cost arising from the excess interfacial area due to defects, the chain mobility, and the activation energy for inter-domain diffusion. The solvent annealing process can be designed to optimize solvent content, fs, to accelerate the assembly. The results shown are applicable to other nanoparticles with different chemical composition and have opened new avenues in designing manufacture-friendly processes, such as draw coating, ink-jet printing, and roll-to-roll processing for the fabrication of nanocomposite-based devices.