Vapor-hydrate equilibria data for the methane + hydrogen + tetrahydrofuran + water system were obtained using the sapphire cell device. The influence of temperature, pressure, initial gas-liquid volume ratio, and the mole fraction of tetrahydrofuran was investigated to evaluate the separation efficiency by forming hydrate at different operating conditions. The experimental results show that decreasing operating temperature or the initial gas-liquid volume ratio and increasing operating pressure or initial tetrahydrofuran mole fraction will be effective to increase the content of hydrogen in the vapor phase. But their influence on the recovery degree of hydrogen in the vapor phase and the operating cost should also be taken into account synthetically when designing a separation process.