Gas hydrates have recently attracted attention due to their potential applications in important not only gas separation/recovery but also the related transportation/storage technologies. In this study, hydrate-based gas separation from CH4/C3H8 gas mixture investigated and evaluated. The phase equilibrium condition of which was predicted using the CSMGem software. Hydrate formation from CH4/C3H8 gas mixture 9.5 % C3H8 at 3.7 MPa and 275.15 K was also investigated to determine the separation efficiency of CH4. During hydrate formation, the vapor phase was analyzed by in situ Raman spectroscopy and double-checked by gas chromatography. The Raman data also revealed the structure of the gas hydrate and the time-dependent encapsulation of guest molecules. The experimental results demonstrated that highly concentrated CH4 can be effectively separated from natural gas hydrates; they will be very useful for methane separation/recovery from natural gas.