We combined the ion-imprinting technique and the binding ability of Fe3+ ions to organosmectite to create the inorgano-organo Fe3+ ions imprinted polymer-nanocomposite traps with the goal of preparing a solid phase that has high selectivity for Fe3+ ions. In the first step, the intercalation of quartamine cations was conducted by an ion-exchange process between the smectite host and an aqueous quartamine solution and Fe3+ ions were complexed with methacryloylamidoantipyrine (MAAP). In the second step, quartamine cations were exchanged with a preorganized metal-chelate complex monomer for the preparation of polymer nanocomposite traps based on the intersurface ion-imprinting. After that, the template ions (i.e., Fe3+) were removed using 4.0 M HNO3 solution. Fe3+-imprinted nanocomposites were characterized by Fourier transform infrared (FTIR), X-ray diffraction (XRD), swelling studies, and elemental analysis. Maximum binding capacity, optimum pH, and equilibrium binding time were found to be 78.5 mg/g, pH 3.0, and 10 min, respectively. The relative selectivity coefficients of the imprinted nanocomposite traps for Fe3+/Al3+, Fe3+/CU2+, Fe3+/ Co2+, and Fe3+/Zn2+ were 5.28, 11.4, 15.8, and 72.6 times greater than the nonimprinted nanocomposites, respectively. The Fe3+-imprinted nanocomposite traps could be used many times without decreasing in their adsorption capacities significantly.