From the view of economic efficiency and technology sustainability, biomass adsorbent has a high potential for pollution control. In the present study, the performance of gemini 12-2-12 surfactant-modified wheat bran (MWB) for the removal of anionic azo dyes from aqueous solution was investigated. A new insight was gained into the modification mechanism through synchrotron-assisted infrared analysis and molecular interaction simulation. The equilibrium and kinetic studies for the adsorption of Acid Red 18 (AR-18), Acid Orange 7 (AO-7) and Acid Black 1 (AB-1) on MWB were conducted. The Langmuir model well fit the adsorption isotherm data. The adsorption kinetics could be described by the pseudo-second-order and intra-particle diffusion models. The results of thermodynamic studies indicated the adsorption of AR-18 and AB-1 onto MWB was endothermic and spontaneous, while the adsorption of AO-7 was exothermic. The optimum pH for the adsorption of anionic azo dyes on MWB was 3. The adsorbed amount of anionic azo dyes onto MWB decreased when NaCl concentration increased from 0 to 0.4 mol L− 1. The potential of modified wheat bran as a suitable adsorbent for the removal of dyes from wastewater was presented in this study. The results can help understand the migration patterns of organic pollutants at wheat bran-water interface. © 2017 Elsevier B.V.