Hydrocarbons play an important role in industrial productionses. The separation and purification of hydrocarbons is one of the most important industrial processes. The separation of low carbon hydrocarbon gases is extremely difficult since their physicochemical properties are similar. The minor differences are their molecular size and valence state. The traditional separation methods suffer from the high energy consumption and low efficiency. Metal-organic frameworks show superiority in separations due to their unique properties including high specific surface area, high porosity and controllable structure size. Computational simulation has been widely used in the investigations of adsorption and separation of MOFs since it can describe the adsorption and separation process at the microscopic level. This paper reviews the recent advances in computational simulations for the adsorption and separation of low-carbon hydrocarbons by metal-organic frameworks. The difficulties and future developments in the study of adsorption and separation of low carbon hydrocarbons by metal-organic frameworks have also been discussed.