Solar‐Driven CO ₂ ‐Mediated Upcycling of Waste Plastics Into Value‐Added Syngas and Carbon Nanotubes

ABSTRACT Plastics and CO 2 are two major waste carbon resources, and their management and recycling are attracting increasing attention. CO 2 ‐mediated plastic upcycling represents a promising strategy for the simultaneous transformation of both wastes, yet it still suffers from high energy demand, low efficiency, and limited applicability to diverse plastics. Here, we report a solar‐driven photothermal strategy that enables the efficient and energy‐saving CO 2 ‐mediated reforming of various plastics, including polyolefins, polyesters, copolymers, and their mixtures, into high‐value syngas and carbon nanotubes (CNTs). The process achieves a syngas yield of 165.6 mmol g cat −1 h −1 , an order of magnitude higher than that of conventional thermocatalysis. Within this system, CO 2 acts not only as an oxidant that consumes the hydrogen species released during plastic dehydrogenation, thereby enhancing efficiency and suppressing methanation but also as a carbon feedstock that directly contributes to both gaseous and solid products. This study provides a powerful solution for the valorization of complex plastic wastes and greenhouse gases and offers new insights into solar‐driven chemical transformations toward a circular carbon economy, while further optimization of the H 2 /CO ratio may expand its compatibility with specific downstream applications.