Recently, the treatment of effluent by agricultural waste biomass has significantly attracted wide interest among researchers due to its availability, efficacy, and low cost. The removal of toxic Remazol Brilliant Blue-R (RBBR) from aqueous solutions using HNO3-treated Juglans nigra (walnut) shell biomass carbon as an adsorbent has been examined under various experimental conditions, such as initial pH, adsorbate concentration, adsorbent dosage, particle size, agitation speed, and type of electrolyte. The experiments are designed to achieve the maximum dye removal efficiency using the response surface methodology (RSM). The optimum pH, adsorbent dosage, and particle size were found to be 1.5, 7 g L−1, and 64 μm, respectively for maximum decolorization efficiency (98.24%). The prepared adsorbent was characterized by particle size, Brunauer–Emmett–Teller (BET) surface area, pore volume, zero-point charge (pHzpc), Fourier transform infrared spectroscopy (FT-IR), field emission scanning electron microscopy/energy dispersive X-ray spectroscopy (FE-SEM/EDX), X-ray diffraction (XRD), and thermogravimetric analysis (TGA). Based on fitting the experimental data with various models, the isotherm and kinetic mechanism are found to be more appropriate with Langmuir isotherm and pseudo-second-order kinetics. The adsorption mechanism can be described by the intra-particle diffusion model, Bangham, and Boyd plots. The overall rate of adsorption is controlled by the external film diffusion of dye molecules. The maximum monolayer adsorption capacity, (qmax) 54.38 mg g−1 for RBBR dye, was obtained at a temperature of 301 K. From a thermodynamic standpoint, the process is endothermic, spontaneous, and the chemisorption process is favored at high temperatures. Desorption studies were conducted with various desorbing reagents in various runs and the maximum desorption efficiency (61.78% in the third run) was obtained using the solvent methanol. Reusability studies demonstrated that the prepared adsorbent was effective for up to three runs of operation. The investigation outcomes concluded that walnut shell biomass activated carbon (WSBAC) is a cost-effective, eco-friendly, and bio-sustainable material that can be used for synthetic dye decolorization in aqueous media.