To evaluate the potential use of two montmorillonite-(Ce or Zr) phosphate crosslinked compounds in removing organic pollutants such as aniline, p-toluidine, and p-acetylaniline from water, adsorption experiments were performed under conditions of varied temperature (288 and 308 K), Adsorption on the montmorillonite-Ce-phosphate compound was best described by a hyperbolic (H-type) isotherm, whereas for the montmorillonite-Zr-phosphate compound, S-type isotherms were obtained for p-toluidine and aniline and L-type for p-acetylaniline. Amines adsorption increases with increasing temperature on the cerium crosslinked material, while for the zirconium-crosslinked compound, adsorption decreases as temperature increases from 288 to 308 K, possibly due to a mainly physical process. Fourier-transform infrared (FTIR) spectroscopy indicated that at the pH generated by the adsorbents, the protonated species of these amines plays an important role in the adsorption process. X-ray diffraction analysis skewed that the aromatic amines are intercalated into the adsorbents. For any given amine, the cerium-montmorillonite adsorbent shows a higher capacity of adsorption compared with zirconium-montmorillonite adsorbent, so it might be reasonably used in removing aromatic amines from water.