This study successfully synthesized a new Metal‐Organic Framework (MOF) named CJLU‐L2, which was constructed from phosphorus‐containing ligands and Co(II) ions. The structure revealed through single‐crystal X‐ray diffraction (SCXRD), features a double‐walled honeycomb‐shaped structure with a one‐dimensional channel of ~ 6.5 Å. According to the PLATON calculation, the pore volume per unit cell of CJLU‐L2 was determined to be 6825.0 Å3, constituting 57.5% of the total crystal volume (11874.9 ų). The Brunauer‐Emmett‐Teller (BET) surface area of CJLU‐L2 was determined to be 954 m²/g by N2 adsorption measurement at 77 K. The phase purity of CJLU‐L2 was verified by powder X‐ray diffraction (PXRD) and infrared spectroscopy (IR), while its thermal stability was confirmed by thermogravimetric analysis (TGA). Hydrogen adsorption experiments demonstrate that CJLU‐L2 exhibits a high hydrogen adsorption capacity, indicating significant potential for gas adsorption applications.