Heterostructured composites with outstanding photocatalytic performance have attracted intense attention because of their great potential for use in environmental remediation. Herein, a facile hydrothermal method to obtain heterostructured composites consisting of graphitic-carbon nitride (g-C₃N₄) and an Fe-based metal organic framework (MIL-101(Fe)) is reported. The as-prepared hybrids exhibited dramatically improved photocatalytic performance for bisphenol A (BPA) degradation in the presence of persulfate (PS) under visible light irradiation. The apparent rate constant, k, for BPA degradation by g-C₃N₄/MIL-101(Fe) composites with PS was approximately 8.9 times higher than that obtained with bare g-C₃N₄. The superior performance arises from the heterojunction formed between MIL-101(Fe) and g-C₃N₄ with a favourable band position and the excellent PS activation ability of MIL-101(Fe), which not only enables the fast electron transfer from g-C₃N₄ to MIL-101(Fe) but also accelerates PS activation for SO₄˙⁻ radical production. This work provides an effective way for constructing novel photocatalytic systems with efficient activity for refractory pollutant removal.