Excessive discharge of synthetic azo dyes into the aquatic ecosystem is a global concern. Here, we develop a green approach to remediate dye pollutants by fabricating an easily separable bio-nanocomposite, based on nanofibrils from whey protein concentrate together with montmorillonite. The nanocomposite was characterized using scanning electron microscopy, Fourier transform infrared spectroscopy, X-ray diffraction and surface area analysis. Nanofibrils lead to a uniform dispersion of montmorillonite in the matrix and also reinforce the nanocomposite. The adsorption efficacy was monitored using cationic (Chrysoidine-G, Bismarck brown-R), reactive (reactive black-5, reactive orange-16), acidic (acid red-88, acid red-114) and direct (direct violet-51, Congo red) dyes. The nanocomposite adsorbed different dyes with different kinetics, cationic dyes quicker and reactive dyes slower. Greater than 93% of Chrysoidine-G was adsorbed over a wide range of dye concentration and pH. Acidic pH and higher temperature are more favorable for the process. Equilibrium adsorption data were reasonably fitted with a linear (Nernst) isotherm model indicating the existence of an unlimited number of adsorption sites which is consistent with the high experimental uptake of 731 mg/g. Kinetic data were well-described by pseudo-second-order and intra-particle diffusion models. We conclude that this environmentally friendly nanocomposite has good potential for use in wastewater treatment and related purposes.