To solve the problem of dehydration in natural gas purification, several MOFs and zeolite molecular sieve membranes has been proposed. Behaviors of adsorption and diffusion for H2O in Natural Gas on HKUST-1 or LTA and T-Type Zeolite Molecular Sieve Membrane were investigated by grand canonical Monte Carlo (GCMC) method. It is found that the classical force fields are not suitable for the system of adsorptions of H2O in Natural Gas on these membranes. The optimized force field parameters were obtained by fitting the experimental data. Results showed that strong competitive adsorption behavior existed in HKUST-1 or LTA and T-Type zeolite for H2O/CH4 mixture. Water loading increased with water content of feed, it was in agreement with the trend of permeation flux for pervaporation dehydration. The diffusivity of pure water molecules was greater than that of pure CH4 . Furthermore, the diffusion behavior of H2O/CH4 mixture through membrane was prominently affected by the interaction between the two components. The CH4 molecules could slow down diffusion of water molecules significantly, thus it would affect permeation flux of these membranes.