<p>Core-shell catalysts have garnered significant attention due to their straightforward control processes, favorable product selectivity, and high added value in the directional or co-production of carbon nanomaterials through the catalytic pyrolysis of polypropylene. They exhibit promising application prospects in energy conversion, environmental management, and chemical synthesis. This paper reviews the utilization of core-shell catalysts in the pyrolysis of polypropylene for the production of carbon nanomaterials, emphasizing their potential for the resourceful utilization of waste plastics. The catalytic performance of core-shell catalysts in the pyrolysis of polypropylene for the synthesis of carbon nanotubes (CNTs) and hydrogen is also detailed. Furthermore, the mechanisms by which parameters such as reactor type, catalyst composition, pyrolysis temperature, reaction atmosphere, and catalyst support influence the distribution and quality of CNTs products are discussed and summarized. The formation mechanisms of catalytic pyrolysis products, along with the existing challenges associated with thermal conversion, are analyzed. This review addresses the development of efficient and cost-effective core-shell catalysts, the optimization of the pyrolysis process, issues related to catalyst deactivation and carbon deposition, and the expansion of CNTs application potential in emerging fields. Future research will focus on advancing the technology for large-scale continuous production of core-shell catalysts, establishing a structure-activity relationship database for carbon nanomaterials, and exploring their application in high-end domains such as new energy storage and flexible electronics. This paper aims to provide theoretical and technical references for the engineering practices related to the catalytic pyrolysis of waste plastics.</p>