Defect construction and heteroatom doping are effective strategies for improving photocatalytic activity of carbon nitride (g-C₃N₄). In this work, N defects were successfully prepared via cold plasma. High-energy electrons generated by plasma can produce N defects and embed sulfur atoms into g-C₃N₄. The N defects obviously promoted photocatalytic degradation performance that was 7.5 times higher than that of pure g-C₃N₄. The concentration of N defects can be tuned by different power and time of plasma. With the increase in N defects, the photocatalytic activity showed a volcanic trend. The g-C₃N₄ with moderate concentration of N defects exhibited the highest photocatalytic activity. S-doped g-C₃N₄ exhibited 11.25 times higher photocatalytic activity than pure g-C₃N₄. It provided extra active sites for photocatalytic reaction and improved stability of N defects. The N vacancy-enriched and S-doped g-C₃N₄ are beneficial for widening absorption edge and improving the separation efficiency of electron and holes.