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Plasma-catalytic pyrolysis was developed for upgrading polypropylene (PP) pyrolysis volatiles to co-produce carbon nanotubes (CNTs) and hydrogen. To uncover the role of plasma on the plastic catalytic pyrolysis process, the pyrolysis of polypropylene (PP) over Fe/γ-Al 2 O 3 was carried out in a two-stage pyrolysis system with a coaxial dielectric barrier discharge (DBD) plasma reactor. The results showed that the plastic pyrolysis volatiles were further cleaved and activated with plasma, resulting in more active carbon species for the growth of CNTs. Compared to conventional catalytic pyrolysis, plasma addition shifted the initial formation temperature of CNTs to a lower ambient temperature by ∼100 °C, and significantly promoted the conversion of liquid and gaseous products to CNTs and hydrogen, with higher carbon and hydrogen yields of ∼322 mg/g plastic and 30 mmol/g plastic , respectively. In addition, the degree of graphitization of the CNTs in the presence of the plasma was significantly enhanced with less defectivity. The influence of catalytic temperature variation caused by plasma on CNTs growth was also discussed from the perspective of volatile evolution. This work highlights the potential of plasma-catalytic pyrolysis for the production of hydrogen and high-value carbon materials from plastic waste. • Plastic was converted into CNTs and H 2 with yields of 322 mg/g plastic and 30 mmol/g plastic , respectively. • Plasma shifted the initial formation temperature of CNTs to lower temperature by ∼100 °C. • The effect of catalytic temperature on plastic pyrolysis volatiles was studied using APPI HRMS. [ABSTRACT FROM AUTHOR]