The remove of the organic pollutants in water plays an important role on the environmental protection, thus photocatalysis, as an effective method, has been attained much attention to deal with this problem. In this paper, a composite of g-C3N4 and Mg-Al hydrotalcite derived metal oxides was prepared to degrade these organic pollutants by simple calcination and co-precipitation methods. And Mg-Al hydrotalcite derived metal oxides were successfully coated on the surface of g-C3N4. The photocatalytic degradation rate of methylene blue reached 97.3% within 1h under visible light, and the degradation rate constant was 0.0432min-1, which is 3.6 times that of g-C3N4. In the recycling process of the catalyst, the good stability of photocatalytic degradation was found. Though characterization analysis, more active sites are exposed to absorb more organic pollutants on the mater surface in the presence of the interinserted and coated structures of composite materials, and the "face to face" contact structure between 2D materials is formed to promote the separation of photogenerated carriers. In addition, the photocatalytic degradation mechanism of the catalyst was explained by free radical scavenging experiment. The material provides an effective method for removing organic pollutants in water, and has broad application prospects.