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High‐temperature proton‐exchange‐membrane fuel cells (HT‐PEMFCs) can offer improved energy efficiency and tolerance to fuel/air impurities. The high expense of the high‐temperature proton‐exchange membranes (HT‐PEMs) and their low durability at high temperature still impede their further practical applications. In this work, a phosphoric acid (PA)‐doped porous aromatic framework (PAF‐6‐PA) is incorporated into poly[2,2′‐(p‐oxydiphenylene)‐5,5′‐benzimidazole] (OPBI) to fabricate novel PAF‐6‐PA/OPBI composite HT‐PEMs through solution‐casting. The alkaline nitrogen structure in PAF‐6 can be protonated with PA to provide proton hopping sites, and its porous structure can enhance the PA retention in the membranes, thus creating fast pathways for proton transfer. The hydrogen bond interaction between the rigid PAF‐6 and OPBI can also enhance the mechanical properties and chemical stability of the composite membranes. Consequently, PAF‐6‐PA/OPBI exhibits an optimal proton conductivity of 0.089 S cm−1 at 200 °C, and peak power density of 437.7 mW cm−2 (Pt: 0.3 mg cm−2), which is significantly higher than that of the OPBI.   The PAF‐6‐PA/OPBI provides a novel strategy for the practical application of PBI‐based HT‐PEMs.

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Development of a perovskite-like metal oxide (PLMO) photocatalyst with a visible light response has long been pursued in the field of photocatalysis. Herein, a PLMO KCuTa 3 O 9 (KCTO) photocatalyst with a narrow band gap of 2.68 eV and a suitable energetic position that straddles the water redox potential has been developed. Subsequently, a 3 nm-thick carbon layer was coated uniformly on the surface of KCuTa 3 O 9 (KCTO@C). The optimized KCTO@C-10 photocatalyst exhibits an excellent photocatalytic hydrogen evolution rate under visible light irradiation (λ > 420 nm), which is 2.87 times higher than that of pure KCTO. Systematic investigations reveal that carbon layer coating on the surface of KCTO not only expands visible light absorption but also promotes electron transfer, facilitating photoinduced electron−hole separation. In addition, an unobvious structural change of the KCTO@C-10 photocatalyst after four cycle tests demonstrates its good photochemical stability. This work offers a perspective for exploiting carbon-coated perovskite-like metal oxide photocatalysts to achieve high-efficiency photocatalytic hydrogen evolution.