A novel kind of solid amine-containing fibrous adsorbent (PP-GMA-TETA) was prepared through irradiation grafting copolymerization with glycidyl methacrylate (GMA) onto polypropylene (PP) fiber, followed by reacting with triethylenetetramine (TETA) to introduce primary and secondary amine groups on its surface. The effects of the reaction conditions, such as the TETA concentration, temperature, and reaction time on amination degree of PP-GMA-TETA, were investigated. Adsorption capacity of PP-GMA-TETA with 77.7% amination degree could reach 4.72 mmol/g. After adsorption, the spent fiber could be completely regenerated at 100 °C by steam for 20 min and its adsorption behavior kept almost constant within six recycles. The comparison of adsorption capacities of amine fibers aminated with various aminating agents also demonstrated that fibers with higher content of primary amine would obtain faster adsorption rates and higher adsorption capacities.