In this study, composite photocatalysts were produced from NiTiO3 and N2-rich precursors (dicyandiamide, melamine, urea, and thiourea) under N2 flow conditions. The goal of the study was to investigate the interaction between NiTiO3 and the synthesized g-C3N4. The properties of the g-C3N4/NiTiO3 (CNT) composites were different depending on the starting materials. Dicyandiamide and thiourea created strong connections with NiTiO3 and resulted in the generation of Ti-N and Ti-O-S bonds. Urea and melamine, however, had difficulty forming g-C3N4 structures or interconnections with NiTiO3. The Ti-N and Ti-O-S bridges in the composite photocatalysts led to increased photocatalytic activity as well as inhibition of the recombination rate. Additionally, the band diagrams of g-C3N4 prepared from dicyandiamide and thiourea exhibited positions suitable for the Z-scheme charge-transfer model with NiTiO3, implying that the composite photocatalysts were applicable for photocatalytic degradation of organic contaminants under the visible-light irradiation. Higher reaction rate constants for the composites prepared with dicyandiamide and thiourea confirmed the significant role of the Ti-N/Ti-O-S bridge between g-C3N4 and NiTiO3.