The coexistence of organic and inorganic pollutants in industrial wastewater has emerged as a concerning environmental issue worldwide due to the critical levels of biological toxicity of these pollutants. In this context, the present study proposes a sandwich structure of fulvic acid and PMIDA-modified LDHs (FA/PMIDA-LDHs) for the simultaneous removal of Cu(2+ )and aniline from wastewater. The specific structure was synthesized using a combination of coprecipitation and impregnation methods. Abundant benzene rings and oxygen-containing functional groups greatly increased the number of sites for the adsorption of both Cu2+ and aniline. The maximum adsorption capacity of Cu2+ and aniline in solution with initial pH 5.0 at 25 ? could reach 221.24 and 132.28 mg/g, respectively. Cu(2+ )could be chelated by the functional groups in the FA/PMIDA-LDHs structure, and a coupled reduction-complexation mechanism was proposed for this process. The uptake of aniline on FA/ PMIDA-LDHs was demonstrated to be a result of the combination of coordination forces, hydrophobic effects, pi-pi interactions, and hydrogen bonds. In a multicomponent solution, FA/PMIDALDHs exhibited excellent salt tolerance of up to 1000 mg/L of Na+ or Ca2+. The effects of Fe3+, Ni2+, Cl-, Cr2O72-, SO42-, and H2PO4- on the uptakes of Cu2+ and aniline were also investigated.