A series of ultra-light aerogels made of oxidized carbon nanotubes and cross-linked polyvinyl alcohol has been prepared by freeze drying of hydrogels, characterised, and tested as amine impregnated solid supports for CO2 capture. The prepared spongy aerogels have demonstrated mechanical, chemical and thermal stability, and are electrically conducting. Polyethyleneimine impregnated aerogels with amine content 75-83% demonstrated CO2 capacity values ≥3.3 mmol/g in a dilute gas stream, which makes the prepared aerogels highly promising supports for amine impregnation in carbon capture applications