CH4 storage associated with adsorbed natural gas (ANG) technology is an issue attracting great concern. Following the Advanced Research Project Agency-Energy (ARPA-E) targeted deliverable capacity of 315 cm3?cm?3 (STP), hundreds of thousands of materials have been experimentally or theoretically evaluated, while the best results still show a 35％gap from the target. Moreover, recent theoretical research reveals that the target is beyond the possibility that real materials can be designed. To get rid of the awkward situation, we make attempts on investigating the CH4 delivery performance under other operation con-ditions. Methods of raising the discharge temperature (to infinite high) or elevating the storage pressure (to 25 MPa) have been proved to show limited effectiveness. In this work, it is found that the ARPA-E tar-get can be achieved by using a decreasing storage temperature strategy. By taking 280 CoRE (computation-ready, experimental) COFs (covalent organic frameworks) as ANG materials, when reduce the storage temperature to 190.6 K, the highest deliverable capacity can reach 392 cm3?cm?3 (STP), and 16.1％ CoRE COFs can surpass the target. The target is also achievable when storage at 220 K. Structure performance relationships study shows strong correlation between deliverable capacity and void frac-tion. Hence, 120 hypothetical COFs are generated to ascertain the optimum void fraction. In addition, the performance of 2D-COFs can be greatly enhanced by increasing the interlayer spacings, e.g. CH4 deliv-erable capacity (storage at 190.6 K) of ATFG-COF can be improved from 239 to 411 cm3?cm?3 (STP) when interlayer spacing is enlarged to 1.65 nm.