In this work, the degradation and mineralization of the non-biodegradable azo dye Orange II (OII) was studied, making use of a heterogeneous Fenton-like oxidation process. For that. hydrogen peroxide activation was achieved by means of two different carbon-based catalysts, which have been impregnated with 7 wt% of iron. The carbon supports employed are quite different, one of them being an activated carbon prepared from agricultural by-products (olive stone), while the other one is a carbon aerogel, prepared by carbonization of an organic resorcinol-formaldehyde polymer. The solids have been characterized using several techniques, namely N-2 and CO2 adsorption at -196 and 0 degrees C, respectively, mercury porosimetry, scanning electron microscopy (SEM), high-resolution transmission electron microscopy (HRTEM), x-ray diffraction (XRD) and x-ray photoelectron spectroscopy (XPS). Then, the catalyst's performance in the Fenton-like oxidation of OII was compared, and the effects of the most relevant operating conditions (pH, catalyst concentration, H2O2 concentration and temperature) analyzed for the most promising one (the carbon aerogel based catalyst). In this catalyst, characterization data point for a very good iron dispersion on the carbon surface. This sample showed very good catalytic performances, with mineralization degrees as high as 90%. However, iron leaching from the support is also considerable leading to a progressive deactivation in consecutive reaction cycles. (c) 2007 Elsevier B.V. All rights reserved.