Fuel cell vehicles powered by hydrogen are particularly attractive and competitive among rapidly developing new energy‐driven automobiles. One critical problem for this type of vehicles is the high cost for hydrogen storage due to the lack of efficient and low‐pressure hydrogen storage technologies. In the frame of development of hydrogen physisorption‐relied materials, attention has mostly been paid to the textural designs of porous materials, including specific surface area, pore volume, and pore size. However, based on the hydrogen physisorption mechanism, hydrogen adsorption energy on a material surface is another key factor with regard to hydrogen uptake capacity. Herein, solid experimental evidences are provided and it is also proven that the chemical states of porous boron nitride (BN) materials remarkably affect their hydrogen adsorption performances. The developed carbon and oxygen co‐doped BN microsponges exhibit the hydrogen uptake capacity per specific surface area of 2.5–4.7 times larger than those of undoped BN structures. These results show the importance of chemical state modulations on the future designs of high‐performance hydrogen adsorbents based on physisorption approaches.