g-C3N4/TiO2 composite has excellent photoelectric properties and is considered as a good carrier of nanoparticles. A novel composite of nZVI-g-C3N4/TiO2 was successfully synthesized through in-situ growth nZVI on the surface of g-C3N4/TiO2 with liquid phase reduction method. The composite was characterized by TEM, XRD, EDS and evaluated its nitrate removal efficiency. The effects of composite dosage, solution initial pH and HCOOH concentration on nitrate reduction were investigated. The results showed that nitrate was rapidly reduced by nZVI-g-C3N4/TiO2 composite. The dosage of 4 g/L nZVI-g-C3N4/TiO2 composite and 3.0 mM of HCOOH concentration was more suitable for nitrate reduction. Solution initial pH had little impact on the nitrate reduction efficiency, but affected the proportion of the nitrate reduction products. The mechanism of nitrate reduction in the nZVI-gC3N4/TiO2/HCOOH-Xe-lamp system was proposed. The nZVI-gC3N4/TiO2 composite could be considered as a viable and promising technology for water pollution remediation.