Measuresbeneficial to enhancing the hydro-stability of the HKUST-1 and improving its adsorptive performance for methane are crucial to the further application. In this research, incorporation of graphene oxide (GO) and carbonization were employed to achieve these objectives. Incorporation of the HKUST-1 was solvothermally prepared by mixing the GO with different mass ratios, and carbonization of the HKUST-1 sample was conducted at different temperatures. Structural characterization, structural morphology observation and adsorption equilibrium measurement of methane were then performed on the samples. Analysis of adsorption equilibrium of methane on the composite was finally carried out within temperature-pressure range respectively about 303.15 K–323.15 K and 0–3.6 MPa. It shows that the sample incorporated by 5 wt% GO has the largest increment about 11.7% and 13.3% in specific surface area and specific micropore volume, and the carbonization conducted at a temperature higher than 300 °C had negative effect on the structure stability of the sample. Results also reveal that the mean relative error between the experimental data and those predicted by Toth equation is about 0.54%. It suggests that the temperature for carbonizing should be carefully selected to avoid the collapse of the structure, and the balance measures should be taken to safeguard the benefit from incorporating.