ordered molecules in a wide variety of morphologies, such as fibers, sheets, and nanotubes. [1,2] Since their independent discovery by Jelley and Scheibe in 1936, [3,4] there has been keen interest in understanding supramolecular assemblies for their unique exciton properties which are distinctly different from those of the single constituting molecules. Close and highly ordered packing allows strong long-range excitonic interaction between the chromophores, resulting in optical properties that strongly depend on the precise alignment of transition dipole moments in the aggregate. In particular, the head-to-tail arrangement of transition dipole moments in J-aggregates leads to the formation of new molecular excitons with redshifted and narrowed spectra. [5] As in natural lightharvesting complexes, molecular excitons in supramolecular assemblies, also called Frenkel excitons, are delocalized over several chromophores in the aggregates. At low temperatures, exciton delocalization lengths of up to 200 molecules have been observed. [6,7] The collective nature of excitations in supramolecular assemblies is responsible for their unique optical properties, such as remarkably narrow and intense absorption, long-range exciton transport, and short radiative lifetimes.As a result of coherent exciton coupling, the oscillator strength for certain excitonic transitions in J-aggregates increases nonlinearly with the number of coupled molecules, leading to strong absorption. In fact, J-aggregates are some of the strongest absorbers known, with measured absorption constants as high as 10 6 cm −1 and absorption strengths reaching 30% at their resonance wavelengths even for a single monolayer. [8,9] Because of their absorption and transport properties, J-aggregates have been widely used as spectral sensitizers in the photographic film industry. [1,2,10] Coherent exciton coupling also leads to a cooperative emission, known as superradiance, which occurs at much faster timescales since the radiative rate is proportional to the oscillator strength. [1,11,12] Even at room temperature, radiative lifetimes as low as 27 ps have been observed for high-quality 2D monolayers of perylene bisimide J-aggregates in the solid state. [9] Because of their strong absorption and superradiant emission, molecular J-aggregates hold great promise towards efficient high-speed light sources, which are important for many applications including high-speed Three general effective strategies are shown to mitigate nonradiative losses in the superradiant emission from supramolecular assemblies. J-aggregates of 5,5′,6,6′-tetrachloro-1,1′-diethyl-3,3′-di(4-sulfobutyl)-benzimidazolocarbocyanine (TDBC) are used to elucidate the nature of nonradiative processes. Selfannealing at room temperature (RT), photo-brightening, and purification of the dye monomers are shown to all lead to substantial increases in emission quantum yields (QYs) and a concomitant lengthening of the emission lifetime, with purification having the largest effect. Structural and optical measuremen...