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The pristine carbon nitride derived from the thermally-induced polymerization of nitrogen-containing precursors(e.g.cyanamide,dicyanamide,melamine and urea)displays low crystallinity because of the predominantly kinetic hindrance.Herein,we reported a modified molten-salts method to fabricate the crystalline carbon nitride under ambient pressure,which is expected to the large-scale production of crystalline carbon nitride.The obtained crystalline carbon nitride displayed about 3.0 times higher pho-tocatalytic NO removal performance than that of pristine carbon nitride under visible light irradiation(λ＜400 nm).Detailed experimental characterization and theoretical calculation revealed the crucial roles of crystallinity in crystalline carbon nitride for the enhanced photocatalytic NO removal performance.This research provided deep insights into the crystallinity of carbon nitride for the enhanced photocatalytic performance.