Efficient utilization of near-infrared (NIR) light that takes a primary percentage of the solar spectrum is of great significance for practical applications of photocatalysis. However, development of singular NIR-based photocatalysts still remains a grand challenge. Herein, a NIR-based crystalline carbon nitride photocatalyst is proposed by using a molten-salt assisted protocol with carbohydrazide as the oxygen-containing precursor. Different from the doping strategy that always leads to structural damage and crystallinity decrease, structural oxygen arising from the special precursor itself is introduced into the framework of C 3 N 4 with highly crystalline structure formed. The n→π* excitation is therefore activated with the absorption edge extended remarkably to 1400 nm. Theoretical calculations also reveal that the local internal electric field is simultaneously generated for promoting the charge separation/migration kinetics. Benefiting from structural oxygen incorporation and crystalline structure formation, the synthesized material shows a significantly enhanced visible-light (λ > 420 nm) hydrogen production reactivity compared with the benchmark carbon nitride, and more importantly an active NIR hydrogen generation (λ > 700 nm) and long-wavelength overall water splitting (λ = 600 nm) capability that is rarely reported for singular photocatalysts. This study showcases an illustration of promising singular NIR photocatalysts for efficient solar fuel production.

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Heteroatom‐doped‐carbon with high electrochemical performance is crucial for the development of advanced carbonaceous materials for energy use. However, achieving homogeneous doping while maintaining electrochemically active microstructure remains challenging. Herein, a feasible hydrothermal protocol to fabricate uniformly N‐doped carbon spheres by in‐situ treatment of glucose and melamine was shown. Melamine served as the soft template to introduce heteroatom dopants while releasing gases to enrich the porous structure. Profiting from the structural directing effect of melamine along with an effective fabrication route, the as‐prepared material presented multiple electrochemically advantageous features including a high surface area, a hierarchical porous structure at different levels, abundant heteroatom doping, etc., and thus delivered high supercapacitance. This work provided an effective strategy for fabrication of carbonaceous scaffold for advanced heterostructured energy materials.