Efficient, atmospheric CO2 capture can act as a renewable source of raw materials as well as a negative CO2 emission. The environmentally friendly and sustainable HighPerCell® process (ionic liquid spun cellulose filaments) allows the spinning of trilobal-shaped cellulose fibers with a large surface area, which provide a favourable carrier material for the subsequent coating with branched Poly(ethyleneimine) (PEI). PEI immobilized on carrier materials are valuable alternatives to aqueous amine solutions for CO2 capture from the atmosphere since the thermal desorption of CO2 from these materials usually requires less energy.