Several nickel-based catalysts (Ni/Al 2 O 3 , Ni/MgO, Ni/CeO 2 , Ni/ZSM-5, Ni-Al, Ni-Mg-Al and Ni/CeO 2 /Al 2 O 3 ) have been prepared and investigated for their suitability for the production of hydrogen from the two-stage pyrolysis–gasification of polypropylene. Experiments were conducted at a pyrolysis temperature of 500°C and gasification temperature was kept constant at 800°C with a catalyst/polypropylene ratio of 0.5. Fresh and reacted catalysts were characterized using a variety of methods, including, thermogravimetric analysis, scanning electron microscopy with energy dispersive X-ray spectrometry and transmission electron microscopy. The results showed that Ni/Al 2 O 3 was deactivated by two types of carbons (monoatomic carbons and filamentous carbons) with a total coke deposition of 11.2wt.% after reaction, although it showed to be an effective catalyst for the production of hydrogen with a production of 26.7wt.% of the theoretical yield of hydrogen from that available in the polypropylene. The Ni/MgO catalyst showed low catalytic activity for H 2 production, which might be due to the formation of monoatomic carbons on the surface of the catalyst, blocking the access of gaseous products to the catalyst. Ni-Al (1:2) and Ni-Mg-Al (1:1:2) catalysts prepared by co-precipitation showed good catalytic abilities in terms of both H 2 production and prevention of coke formation. The ZSM-5 zeolite with higher surface area was also shown to be a good support for the nickel-based catalyst, since, the Ni/ZSM-5 catalyst showed a high rate of hydrogen production (44.3wt.% of theoretical) from the pyrolysis–gasification of polypropylene.