Covalent organic frameworks (COFs) possess good porosity, uniform channels, and tunable skeletons, as well as excellent stability, which are well-suited for gas adsorption. In this study, we developed two pyrazine-based COFs, namely, TFPPz−MPA−COF and TFPPz−BD(OMe) 2 −COF, by condensation reaction of C 4 and C 2 axisymmetric monomers. Both COFs exhibited good crystallinity, well-defined pore structures, and outstanding thermal and chemical stability. TFPPz−MPA−COF and TFPPz−BD(OMe) 2 −COF demonstrated high iodine adsorption capabilities of up to 5.41 and 5.18 g g −1 in iodine vapor, and 95.42 and 98.04 mg g −1 in n-hexane, respectively. In addition, TFPPz−MPA−COF and TFPPz−BD-(OMe) 2 −COF exhibited good CO 2 uptake capacities of 1.48 and 1.34 mmol g −1 at 273 K, respectively.