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Here, a dual regulation strategy to construct nitrogen vacancies-modified and metal-free group-intercalated g-C 3 N 4 (NP–CN) photocatalyst is proposed. The nitrogen vacancies in the planes of NP-CN could adjust the band-gap of CN, while the metal-free group intercalated between layers act as electron transport channels for fast charge carrier separation. The nitrogen vacancies as well as metal-free group intercalate significantly increase the photocatalytic performance in H 2 evolution and dye degradation. The photocatalytic H 2 evolution rate and apparent first-order rate constant for RhB removal of NP-CN24 is 22 and 7.3 times higher than that CN, respectively. This work provides a facile approach to design and synthesize new modification of CN photocatalyst via nitrogen vacancies and metal-free group intercalation to simultaneously improve the activity in the photocatalytic application field. • Nitrogen vacancies-modified and metal-free group-intercalated g-C 3 N 4 (NP–CN) is prepared. • NP-CN shows high activity and stability in photocatalytic H 2 evolution and dye degradation. • The photocatalytic H 2 evolution activity of NP-CN is 22 time that of the pristine g-C 3 N 4. [ABSTRACT FROM AUTHOR]