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A well-ordered highly crystalline g-C 3 N 4 nanorods (CNR) is rationally tailored by molten salt-assisted anti-defect engineering for efficient artificial photosynthesis of H 2 O 2. [Display omitted] • Highly crystalline and well-ordered g-C 3 N 4 nanorods are tailored. • Molten salt-assisted preparation of highly crystalline organic polymeric materials. • Anti-defect engineering promotes charge separation and transfer. • The H 2 O 2 generation rate reaches 1.58 mmol g-1h−1 only using air as oxygen source. • Molten salt-assisted anti-defect engineering to improve photocatalytic activity. Graphite carbon nitride (g-C 3 N 4) is widely recognized as one of the most popular catalysts for photocatalytic hydrogen peroxide (H 2 O 2) production. However, it is often overlooked that general g-C 3 N 4 materials contain numerous dangling bonds and defects, which serve as recombination centers for photogenerated carriers and significantly hinder their catalytic activity. Herein, we present a novel approach to address this issue by rationally tailoring well-ordered g-C 3 N 4 nanorods (CNR) through molten salt-assisted anti-defect engineering. The resulting highly crystalline CNR demonstrates high efficiency in the artificial photosynthesis of H 2 O 2. Experimental results indicate that enhancing the crystallinity of g-C 3 N 4 while reducing the defect concentration effectively promotes charge separation and transport. As a result, it exhibits a remarkable H 2 O 2 generation rate of 1.58 mmol g-1h−1 using air as the oxygen source, accompanied by an apparent quantum yield of 18.00 % (λ = 400 nm). The excellent photocatalytic performance of CNR surpasses that of all previously reported pristine g-C 3 N 4 materials. This work sheds light on the effectiveness of molten salt-assisted anti-defect engineering in improving catalyst activity, with potential applications in solar cells, sensor devices and other catalytic systems. [ABSTRACT FROM AUTHOR]