This article reports on the preparation of iron nanoparticles (FeNPs) supported in chitosan beads (Chi-EDGE-Fe) for removing aldrin from aqueous solutions. The FeNPs and Chi-EDGE-Fe beads were characterized by means of scanning electron microscopy (SEM), transmission electron microscopy (TEM), X-ray diffraction (XRD), Fourier transform infrared (FTIR), and the Mössbauer spectroscopy (MS) techniques. TEM, XRD, and MS showed that the FeNPs had core-shell structures consisting of a core of either Fe0 or Fe2B and a shell of magnetite. Furthermore, SEM images showed that Chi-EDGE-Fe beads were spherical with irregular surfaces and certain degrees of roughness and porosity, whilst the sorbent mean pore size was 204 nm, and the occluded iron nanoparticles in the chitosan material had diameters of 70 nm and formed agglomerates. The sorbent beads consisted of carbon, oxygen, chlorine, aluminum, silicon, and iron according to the SEM-EDS analysis. Functional groups such as O-H, C-H, -CH2, N-H, C-O, C-OH, and Fe-OH were detected in the FTIR spectra. In addition, a characteristic band appeared at about 1700 cm−1 after the sorption process involving aldrin. MS also showed that the iron nanoparticles in the beads probably oxidized into NPs of α-Fe2O3 as a result of the supporting process. The isotherm of the aldrin removal followed the Langmuir–Freundlich model and presented a maximum adsorption capacity of 74.84 mg/g, demonstrating that chitosan-Fe beads are promising sorbents for the removal of toxic pollutants in aqueous solutions.