Experiments were conducted for developing suitable ANG adsorbents for vehicular applications. MIL-101 and activated carbon samples were respectively prepared by hydrothermal and chemical activation methods. Two samples were undergone structure analysis on adsorption data of nitrogen at 77.15 K, and adsorption data of methane were then volumetrically measured within temperature–pressure range 293.15 K–313.15 K and 0–8 MPa. A conformable vessel in volume 2.5 L was employed for charge/discharge tests under the flow rate 10–30 L·min?1. It shows that limit isostreic heat of methane adsorption is respectively about 25.15 kJ·mol?1 and 22.94 kJ·mol?1 on the activated carbon and the MIL-101, and isosteric heat within the experimental condition is 14–19.5 kJ·mol?1;employing a smaller charge/discharge flow rate can weaken the temperature fluctuation of the adsorbent bed and increase the charge/discharge amount;employing honeycomb heat exchanging device enhance the thermal conductivity of the adsorbent bed by consuming a negligible part of volume of the vessel. It suggests that a smaller flow rate for charge/discharge should be employed, and MOFs together with the honey-comb heat exchanging device are promising for practical applications.