This work demonstrates a strategy for constructing 3D COFs with ultrahigh surface area. The synthesized 3D-TFB-COFs with ultrahigh surface area achieve the target pore size and exhibit an impressive balance between the gravimetric and volumetric methane working capacities at related conditions of ANG, along with high adsorption stability. This research establishes 3D-TFB-COFs as promising absorbents for methane storage and introduces a strategy for the design and synthesis of advanced highly porous 3D COFs.