The spinel Zn2TiO4 single crystals were grown via optical floating zone technology in an argon atmosphere for the first time, the as-grown crystals were dark blue and transparent. And the as-grown crystals, free of bubbles and with low angle grain boundary, grow along the a-axis direction. The annealed crystals were colorless and transparent, and the chemical valence of as-grown and annealed single crystals was characterized by X-ray photoelectron spectra. The room-temperature polarized Raman spectra of spinel Zn2TiO4 crystal were presented and the in situ temperature-dependent Raman spectra of the crystals were also described. DSC results of Zn2TiO4 were also discussed.