Graphitic carbon nitride/bismuth ferrite (g-C 3 N 4 /BiFeO 3 ) nanocomposites with various g-C 3 N 4 contents have been synthesized by a simple method. After the deposition–precipitation process, the novel BiFeO 3 spindle-like nanoparticles with the size of ∼100nm were homogeneously decorated on the surfaces of the C 3 N 4 nanosheets. A possible deposition growth mechanism is proposed on the basis of experimental results. The as-prepared g-C 3 N 4 /BiFeO 3 composites exhibit high efficiency for the degradation of methyl orange (MO) under visible light irradiation, which can be mainly attributed to the synergic effect between g-C 3 N 4 and BiFeO 3 . The ability to tune surface and interfacial characteristics for the optimization of photophysical properties suggests that the deposition growth process may enable formation of hybrids suitable for a range of photocatalytic applications based on g-C 3 N 4 .