Abstract: This study reports the preparation of catalyst grains based on oxyhydroxides of iron and zirconium via the coprecipitation method and their application in the degradation of 4-nitrophenol. The morphology, microstructure, and surface composition of these catalysts were characterized by scanning electron microscopy, X-ray diffraction, nitrogen physisorption, and Fourier transform infrared spectroscopy. The catalytic activity of the grains was assessed in the degradation of 4-nitrophenol in a heterogeneous system at different operating conditions. Degradation rates up to 93% were obtained after 4 h of contact time where the catalytic activity of tested materials was higher at pH 7 than in acidic and basic conditions. Amorphous iron hydroxide with a ratio of 75% Zr+25%Fe showed the best catalytic properties. These novel materials are an interesting alternative for facing the water pollution caused by organic compounds.