This work focuses on the characterization of five palygorskite clays from the Brazilian state of Piaui and their feasibility as eco-friendly adsorbents for the removal of Fe³⁺ ions from aqueous solutions. For characterization, we applied the techniques of X-ray diffraction (XRD), X-ray fluorescence (XRF), scanning electron microscopy with energy dispersive spectroscopy (SEM/EDS), size distribution measurements, density measurement by He pycnometry, superconducting quantum interference device (SQUID) magnetometry, Fourier-transform infrared spectroscopy (FTIR), thermogravimetric analysis (TGA/DTA), zeta potential measurement, hydrophobicity determination by contact angle, Brunauer–Emmett–Teller surface area analysis (BET technique) and atomic force microscopy (AFM). Batch experiments were performed in function of process parameters such as contact time and initial concentration of Fe³⁺. The natural palygorskites (Palys) had excellent performance for the removal of Fe³⁺ from aqueous solutions by adsorption (around 60 mg/g), and the Langmuir is supposedly the best model fitted the experimental data.