Atomically thin 2D carbon nitride sheets (CNS) are promising materials for photocatalytic applications due to their large surface area and very short charge‐carrier diffusion distance from the bulk to the surface. However, compared to their bulk counterpart, CNS' applications always suffer from an enlarged bandgap and thus narrowed solar absorption range. Here, an approach to significantly increase solar absorption of the atomically thin CNS via fluorination followed by thermal defluorination is reported. This approach can greatly increase the visible‐light absorption of CNS by extending the absorption edge up to 578 nm. The modulated CNS loaded with Pt cocatalyst as a photocatalyst shows a superior photocatalytic hydrogen production activity under visible‐light irradiation to Pt‐CNS. Combining experimental characterization with theoretical calculations shows that this approach can introduce cyano groups into the framework of CNS as well as the accompanied nitrogen vacancies at the edges, which leads to both narrowing the bandgap and changing the charge distribution. This study will provide an effective strategy to increase solar absorption of carbon‐nitride‐based photocatalysts for solar energy conversion applications.

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Aluminum‐ion batteries (AIBs) are regarded as one of the most promising types of energy storage device in light of the safety, natural abundance, and electrochemical properties of aluminum. However, the rate capabilities of AIBs are limited owing to the sluggish kinetics of chloroaluminate anions. In this study, a covalent organic framework (COF) is adopted as the cathode material in AIBs. Theoretical and experimental results suggest that the COFs allow fast anion diffusion and intercalation without structure collapse, owing to the robust frameworks and the hierarchical pores with a large specific surface area of 1794 m2 g−1. The resultant AIB exhibits remarkable long‐term stability, with a reversible discharge capacity of 150 mAh g−1 after 13 000 cycles at 2 A g−1. It also shows an excellent rate capability of 113 mAh g−1 at 5 A g−1. This work fully demonstrates the potential of COFs in the storage of chloroaluminate anions and other large‐sized ions.