The study aims to determine the adsorption mechanism of reactive brilliant red X-3B (RBR) on a novel low-cost clay–biochar composite with different proportions of bagasse and natural attapulgite (ATP). Pure bagasse, pure ATP, and two mixtures with weight ratios of 1:5 and 1:3 were pyrolyzed at 700 °C for 4 h in a muffle furnace. Biochar samples were characterized with an element analyzer and by scanning electron microscopy, X-ray diffraction, Fourier transform infrared, X-ray photoelectron spectroscopy, Brunauer–Emmett–Teller method, and zeta potential measurement. Results of the batch and leaching experiments showed that the adsorption capacities followed the order of 1:3 clay–biochar > 1:5 clay–biochar > bagasse biochar > pure ATP. Furthermore, ATP and bagasse exerted a synergistic effect on the adsorption of RBR. The adsorption data showed good correlation with the Langmuir isotherm, and the kinetic data were fitted to the pseudo-second-order model. The adsorption of RBR on clay-biochar involved electrostatic interaction, hydrogen bond, π–π interactions, and surface participation. The modification of biochar by ATP improved the adsorption capacity by increasing functional groups and creating adsorption sites. Therefore, ATP-modified clay–biochar composites could be effective adsorbents for the removal of RBR from wastewater.