Most of the reported composites of g-C3N4/metal-organic frameworks (MOFs) were obtained via exfoliation of g-C3N4 and wrapping the nanosheets on MOFs with weak interaction. In this work, chemical protonation of g-C3N4 and dip-coating was adopted as a feasible pathway to achieve the real combination of g-C3N4 derivatives with a familiar MOF material MIL-100(Fe). Structural, chemical and photophysical properties of the novel hybrid photocatalysts were characterized and compared to those of the parent materials. It was verified that the protonated g-C3N4 species of appropriate content were uniformly coated along the frameworks of MIL-100(Fe) with strong interaction. The optimal materials maintained the intact framework structure, surface property and porosity of MIL-100(Fe), as well as the inherent structural units and physicochemical properties of C3N4. In comparison to the parent materials, the protonated g-C3N4 coated MIL-100(Fe) materials exhibited enhanced photocatalytic activity in degradation of rhodamine B or methylene blue dye, as well as in oxidative denitrogenation for pyridine by molecular oxygen under visible light. Introduction of protonated g-C3N4 on MOFs improved the adsorption ability for contaminant molecules. Furthermore, coating effect provided a platform for rapid photoexcited electrons transfer and superior separation of photogenerated electron-hole pairs. Photocatalytic conversion of the three contaminants followed different mechanisms. (C) 2018 Elsevier B.V. All rights reserved.