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The conversion of waste plastic into high‐value‐added chemicals is regarded as a promising approach for relieving global plastic pollution and contributing to the circular economy. Herein, a partial calcination strategy is developed to fabricate a zinc oxide/UiO66‐NH2 (ZnO/UiO66‐NH2) heterojunction, in which ZnO is encapsulated in porous UiO66‐NH2 for the photocatalytic valorization of plastic. This strategy preserves the framework structure of UiO66‐NH2, thus enabling the formation of ZnO with ultra‐small size distributed inside the skeleton. The synergistic effect of the obtained ZnO/UiO66‐NH2 heterojunction facilitates providing an efficient channel for carrier/mass transfer and guarantees structural stability. As a result, ZnO/UiO66‐NH2 exhibits high activity for converting polylactic acid (PLA) and polyvinyl chloride (PVC) into acetic acid, coupled with H2 production. This work provides a feasible strategy for rationally designing heterojunction photocatalysts, as well as an insight into understanding the process of photocatalytic valorization of plastic.

Unleashing the Power of Photocatalysts for Plastic Upcycling In article 2214839, Wenjing Zhang, Yibo Dou, and co‐workers develop a partial calcination strategy to encapsulate ZnO within the porous UiO66‐NH2 and create an ZnO/UiO66‐NH2 heterojunction. This novel approach significantly enhances the selectivity in photocatalytic valorization of waste plastics into acetic acid, while concurrently generating hydrogen.

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