In this paper, a series of surface-alkalinized graphitic phase carbon nitride (g-C3N4) were synthesized via a one-step strategy employing dicyandiamide as the precursor. The effects of single salts (KCl, NH4Cl) and complex salts (KCl with NH4Cl) on the morphological structure, compositional composition, optical properties, and photocatalytic performance of alkalized CN samples were investigated. The IR and XPS analyses revealed that new structural units, C≡N and (N)2C-OH, were formed in the CN structure, indicating that the surface alkalinization of g-C3N4 had been successful. After in-situ surface alkalinization, the energy band structure of CN was optimized, the light absorption range was widened, and the photocatalytic activity was enhanced. Among them, the compound salt alkalinized sample (CNK2.0) at twice the amount of KCl as dicyandiamide showed the most excellent photocatalytic degradation performance. Its degradation efficiency of methylene blue within 60 min could reach 83.39 %, which was 2.05 times higher than that of pure g-C3N4. With a 47.1 % reduction of Cr(VI) at 60 min, the CNK1.5 sample demonstrated the prime photocatalytic activity, which was 34.2 % higher than that of pure g-C3N4. The surface hydroxylation and the optimization of the energy band structure are the main reasons for the enhanced photocatalytic activity of carbon nitride after complex salt alkalinization.