Eco-friendly carbothermal techniques were used to synthesize nanocomposites of biowaste-derived Ni/NiO decorated-2D biochar. The use of chitosan and NiCl2 in the carbothermal reduction technique was a novelty to synthesize the Ni/NiO decorated-2D biochar composite. Potassium persulfate (PS) was found to be activated by Ni/NiO decorated-2D biochar, which is thought to oxidize organic pollutants through an electron pathway designed by the reactive complexes formed between PS and the Ni/NiO biochar surface. This activation led to the efficient oxidation of methyl orange and organic pollutants. Analyzing Ni/NiO decorated-2D biochar composite before and after the methyl orange adsorption and degradation procedure allowed us to report on the process of its elimination. The Ni/NiO biochar with PS activation showed higher efficiency than Ni/NiO decorated-2D biochar composite as this material was able to degrade over 99% of the methyl orange dye. The effects of initial methyl orange concentration, dosages effect, solution pH, equilibrium studies, kinetics, thermodynamic studies, and reusability were examined and evaluated on Ni/NiO biochar. © 2023 Elsevier Ltd