Magnetic ordered mesoporous carbons (OMCs) with Ni nanoparticle (average size: 10 nm) homogeneously modified on surfaces of OMCs were successfully fabricated via a facile casting route. The microstructure, pore size distribution, pore structure, and surface area of the synthesized OMCs and Ni decorated OMCs (Ni-OMCs) were characterized by X-ray diffraction, field emission scanning electron microscopy, high-resolution transmission electron microscopy and N(2) sorption. The characterization by magnetic hysteresis loops suggests a ferromagnetic behavior for the Ni-OMCs samples with a magnetization saturation of 2.34 emu g(-1) at 300 K. high enough for magnetic separation. The ferromagnetic Ni-OMCs were used as magnetically separable high-performance adsorbents for methyl orange (MO). The adsorption capacities for MO on the Ni-OMCs as magnetically separable adsorbents were investigated comparatively with pristine OMCs and activated carbon powder (ACP). The results show that the adsorption capacities for MO on the OMCs and Ni-OMCs adsorbents could be well described according to Langmuir isotherm with MO molecule preferentially adsorbed in the structured mesopores, suggesting the adsorption type of monolayer coverage of MO dye onto the mesoporous samples. The effects of surface area, pore structure, and the Ni deposition on the adsorption capacities for MO were systematically investigated. The effects of several important parameters such as contact time, temperature, adsorbent dosage and adsorbate concentration on the adsorption capabilities were studied in detail. The ferromagnetic Ni decorated OMCs as adsorbents for MO, were easily dispersed, separated and removed in an external applied magnet field, and can be more convenient for large scale applications than filtration or centrifugation separation route. (C) 2011 Published by Elsevier B.V.