Self-organization in dispersed liquid crystal compounds based on the charge-transfer complexes between an organic donor (monomer, polymer, nanoparticles) and a fullerene has been investigated. 10 μm nematic liquid crystal cells with the fullerene complexes based on 2-cyclooctylamine-5-nitropyridine, polyaniline, and phthalocyanine nanoparticles have been studied. It was found that the exposure in a few days resulted in the self-arrangement of the nematic liquid crustal system with the fullerene complex. The microscopic study allowed the transition to be revealed from the nematic phase to the smectic one. For all structures the switch-on time close to 50-100 μs has been obtained. It follows from our results that the mechanism of the accelerated rotation of the LC dipoles is likely to be caused by the order parameter change during the transition from the nematic to the smectic induced the fullerene-containing complex introduction. The complex formation was supported by the data of absorption and luminescence spectra, mass-spectroscopy, non-linear measurements of light-induced effects, and a quantum-chemical simulation. Potentials of these systems for laser optics, medicine, and display application have been examined.