Single crystal of LiBaB9O15 for the first time has been grown from a Li2Mo3O10 flux by the top-seeded growth method. Details on the preparation and growth procedures are discussed. The phase structure of the as-grown crystal was determined by X-ray powder diffraction (XRD). The frequencies of the vibrational modes of the crystal were obtained from Infrared and Raman spectrum measurements. The results show that the obtained crystal is well-crystallized and indexed as a trigonal crystal system with lattice parameters of a = b=10.95053 , c = 16.88215 , and V = 1753.19 (3). The observed frequencies were assigned on the basis of the BO3 and BO4 vibrations, and correlations with previous data reported for the similar compounds. On the basis of the XRD data and interfacial angle measurements, the as-grown crystal was found to be bounded by the (110), (113), and (101) planes. The seed crystal used for producing the crystal was oriented along the [100] direction.