The high-purity purification of 2,6-dimethylnaphthalene (2,6-DMN, 10.43 wt%) from the concentrate of DMN isomers recovered from light cycle oil (LCO) through distillation-extraction combination was examined by a crystallization operation. To select the most suitable crystallization solvent for purification of 2,6-DMN, several conventional solvents, which have been employed commercially as crystallization solvents for high-purity performance, were tested, through measurement of purity and yield of 2,6-DMN. The solvents used were acetone, cyclohexanone, ethanol, ethyl ether, ethyl acetate, isopropyl ether, methanol, n-hexane, n-heptane, pyridine, THF, toluene, and a mixture of methanol and acetone. The mixture of 60 vol% methanol and 40 vol% acetone (M/A = 1.5) was found to be suitable for purification of 2,6-DMN in the concentrate of DMN isomers based on purity and yield. Increasing the operation temperature and the volume ratio of solvent (M/A = 1.5) to feed (concentrate of DMN) resulted in improving the purity of 2,6-DMN, whereas the yield decreased. The crystal recovered by crystallization run using the concentrate of DMN isomers contained about 76 wt% 2,6-DMN. Furthermore, for recovery of high-purity 2,6-DMN, crystal containing 76 wt% 2,6-DMN was crystallized. As a result, crystal with 99.7 wt% 2,6-DMN was recovered with 40% yield.