Adsorption is an important technique for the separation and purification of various gases. In this study, two types of graphene materials with various morphologies are employed to modify metal-organic frameworks (MOFs) and improve their adsorption capacities. SEM, XRD, as well as Raman and IR spectroscopies are adopted to analyze the microstructures of these as-prepared samples. After the combination process, the adsorption abilities of UiO-66 and ZIF-8 are enhanced significantly (an increase of more than 48% for the n-hexane adsorption), and the adsorption amounts of CO2, methanol, and n-hexane reach 9.32, 17.48, and 4.26 mmol g(-1), respectively. The remarkably improved performances are induced by the more favorable orbit interaction between the graphene basal plane and the adsorbed gases. Moreover, the natural three-dimensional (3D) continuous and porous structure of the 3D graphene network is not only beneficial to the adsorption ability but also improves the stability of MOFs at a high temperature.