Abstract：For the excessive phenomenon of indoor air pollutant formaldehyde, the new carbon nanomaterials (graphene,  carbon nanotubes) were introduced into the field of gaseous pollutants removal. Using the characteristic of graphene solution that forming gel under certain conditions and adopts sponges as skeleton, construct the three-dimensional structure of aerogels of graphene/carbon nanotubes/sponge. Further improve the performance of formaldehyde removal of the carbon nanotube/graphene aerogel (GCNTs/EDA-S) by modified with amino groups and study the adsorption mechanism. The results of experiment show that both of graphene and carbon nanotubes have good adsorption properties after modified with amino functional groups. The breakthrough time of GCNTs/EDA-S can be up to 4024min/g and the maximum adsorption capacity is 13.5mg/g under the formaldehyde concentration of 3.7PPM.