Covalent organic frameworks (COFs) based on pyrene (Py) building blocks have emerged as a promising class of photocatalysts for solar-to-chemical conversion. This review comprehensively summarizes recent advances in the design and application of Py-COFs for two critical reactions: photocatalytic hydrogen evolution and hydrogen peroxide synthesis. We primarily highlight the various functionalized Py monomers for constructing Py-COF photocatalysts. The structural modulation of Py-COFs at multiple levels is followed to enhance their photocatalytic performance. The molecular engineering strategies, such as donor-acceptor construction, heteroatom doping, and linkage modulation, are employed to precisely tailor the optoelectronic properties, band structures, charge separation efficiency, and surface reaction pathways. The synergistic effects of framework-level structural innovations (e.g., dimensionality control, pore engineering), metal doping, and heterojunction construction are discussed for their roles in optimizing mass transport, active site exposure, and interfacial charge dynamics of the solar-to-chemical reaction. A systematic analysis of structure-performance relationships reveals that synergistic integration of multiple design principles is key to overcoming inherent limitations of organic semiconductors. Finally, current challenges and future perspectives are outlined, providing a roadmap for the development of high-performance, stable, and scalable Py-COF photocatalysts to meet the growing demands for sustainable energy and green chemical synthesis.
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