Sr or Ba filled type-I Ge clathrate single crystals were prepared using high pure elemental Ga, Ge, and Sr or Ba as the starting materials, and Ga as a flux. Powder X-ray diffraction (XRD), energy dispersive X-ray spectroscopy (EDS), differential scanning calorimeter (DSC) were used to characterize the crystals, respectively. The results show that large and well-crystallized single crystals can be prepared under optimum synthesis condition. The composition of the crystals is in good agreement with the nominal composition (M8Ga16Ge30, M=Sr, Ba). Raman spectra of the single crystals were studied at room temperature and several of the Raman active vibrational modes in the crystals have been identified.