The environmental crisis caused by excessive emissions of carbon dioxide-based greenhouse gases has garnered widespread public concern. Solid amine is considered to be one of the most effective carbon dioxide (CO2) adsorbents. However, traditional solid amine carriers have problems such as structural collapse, low efficiency and poor regeneration. In this study, waste wool having hierarchical fibrous structure was spunlaced, fibrillated and later compounded with amino acid ionic liquids (AAIL) leading to the formation of the AAIL@feather-like wool nonwoven absorbents. A synergistic co-amine effect was observed after primary and secondary fibrillation without any sacrifice in the mechanical property of wool nonwovens. Also, the fibrillated nonwovens had high specific area which provided high loading rate (13.53 %) on AAIL. Compared with untreated wool nonwovens, the CO2 adsorption capacity of feather-like wool nonwovens was higher by 65 % (11.75 mmol/g) after loading AAIL. Furthermore, the CO2 adsorption capacity was retained (95.2 %) even after 12 cycles at 80 ℃, indicating that the AAIL@ feather-like wool nonwovens possess good long-term stability. This work paves the way for large scale manufacturing of biobased solid adsorbents with a hierarchical nonwoven structure for efficient CO2 capture.