The controlled self-assembly of molecules and interactions between them remain a challenge in creating tunable and functional organic nanostructures. One class of molecular systems that has proven useful for incorporating tunable functionality at different length scales is liquid crystals (LCs) due to its ability to inherently self-organize. Here we present a novel approach to utilize the self-assembly of polymerizable liquid crystals to control the molecular aggregation of stable fluorescent chromophores and create a unique class of organic fluorescent nanocolloids. By adjusting the ratio between the dye and LC molecules inside the nanocolloids, we demonstrate the ability to control the molecular interactions and tune the fluorescent emission spectra of nanocolloid populations under single wavelength excitation. The single absorption spectrum and multiple emission spectra are highly desirable and reminiscent of the spectroscopic signature of quantum dots. These novel fluorescent nanocolloids have broad potential applications in fluorescent imaging and biological labeling.