In this work, the bio-nanohybrids of magnesium-aluminum layered double hydroxide intercalated with zwitterionic histidine (His-LDH) was synthesized. The crystal phase, morphology, and nanostructure of the as-prepared His-LDH were characterized by X-ray diffraction (XRD), scanning electron microscopy (SEM), transmission electron microscopy (TEM), Fourier transform infrared spectroscopy (FT-IR), and nitrogen adsorption-desorption methods. The His-LDHs were used to remove anionic dyes, including Congo red (CR), indigo carmine (IC) and sunset yellow FCF (SY) from aqueous solutions. The detailed investigation of the kinetics and the adsorption isotherms of CR, IC and SY from aqueous solutions showed that the dyes adsorb rapidly, in accordance with a pseudo-second-order kinetics and a Freundlich adsorption isotherm model. The remarkably high adsorption capacity of the dyes on the His-LDH (efficiency of CR removal, 99.98%; maximum specific removal q(max), 1112 mg g(-1); efficiency of IC removal, 98.98%; q(max), 625 mg g(-1); and efficiency of SY removal, 99.78%; q(max), 400 mg g(-1)) is rationalized on the basis of electrostatic interactions as well as pi-pi and H-bonding interactions between the His-LDH adsorbent and the acidic dyes. Adsorption experiments indicate that the resulting His-LDH has great potential applications as an environmentally friendly material for the swift removal of acidic dyes from aqueous solutions. (C) 2018 Elsevier Inc. All rights reserved.