The invention provides a method for modifying a covalent organic framework material. The method comprises the following steps: (1) mixing 1,3,5-tris-(4-aminophenyl)benzene with 2,5-dioxymethyl-terephthalaldehyde, adding o-dichlorobenzene/n-butanol and an acetic acid catalyst, carrying out freezing-exhausting-unfreezing circulation for several times, carrying out flame sealing, heating, centrifugally collecting precipitates, washing, carrying out Soxhlet extraction, drying, and collecting powder, so as to obtain TPB-DMTA-COF; (2) adding 2-methyl-2-butene, a sodium chlorite water solution and glacial acetic acid into dioxane suspension liquid of the TPB-DMTA-COF powder, and stirring in a dark environment, so as to obtain purple solids; and (3) re-oxidizing the purple solids by virtue of thesodium chlorite water solution, and carrying out filtration separation, washing, drying, so as to obtain purple powder. The preparation method is simple, the synthesis conditions are easily controlled, and prepared O-TPB-DMTA-COF powder has a good glycopeptides enriching effect.