The economic cleanup of wastewater continues to be an active area of research. In this study, the influence of pore size on regeneration by Fenton oxidation for carbon materials with adsorbed methyl orange (MO) was investigated. More specifically three carbon supports, with pore sizes ranging from mainly microporous to half microporous-half mesoporous to mainly mesoporous, were impregnated with γ-Fe2O3 to make them magnetic and easy to separate from solution. The carbon samples were characterized before adsorption and after regeneration with hydrogen peroxide at 20 °C. In addition, adsorption kinetics and isotherms were collected, and the Weber-Morris intraparticle diffusion model and Freundlich isotherm model fit to the data. The adsorption capacity increased with increasing microporosity while the regeneration efficiency increased with increasing mesoporosity. Further experiments with varying regeneration and adsorption conditions suggested that the regeneration process may be kinetically limited. The MO adsorbed in the micropores was strongly adsorbed and difficult to remove unlike the MO adsorbed in the mesopores, which could be reacted under relatively mild conditions. Thus, there was a trade-off between adsorption capacity and regeneration.