Magnetic Fe/Ni nanoparticles doped bimodal mesoporous carbon (MBMC) was prepared for highly effective adsorption of cationic dye methylene blue (MB) and anionic dye methyl orange (MO). Structure characterization demonstrated that Fe/Ni nanoparticles were embedded into the interior of the mesoprous carbon, and MBMC maintained ordered and bimodal mesopores. The effects of several parameters such as contact time, pH, temperature, ionic strength and dye molecular structure on the adsorption were investigated. Alkaline pH was better for MB adsorption, while acidic pH was more favorable for MO uptake. The adsorption capacity was slightly enhanced when existing ion concentrations increased. Adsorption on MBMC was affected by the molecular structures of different dyes, and both primary and secondary pores of MBMC were involved in dye adsorption. The adsorption kinetics fitted well with pseudo-second-order model and exhibited 3-stage intraparticle diffusion mode. Equilibrium data were best described by Langmuir model, and the estimated maximum adsorption capacity for MB and MO was 959.5 mg/g and 849.3 mg/g, respectively. Thermodynamic studies indicated that the adsorption process was spontaneous and endothermic. Moreover, the adsorbent could be regenerated using ethanol, and the regenerated adsorbent after seven cycles could retain over 80% of the adsorption capacity for the fresh adsorbent. The results suggested that MBMC could be considered as very effective and promising materials for both anionic and cationic dyes removal from wastewater. (C) 2015 Elsevier Inc. All rights reserved.