It was shown for the first time that the efficiency of dye adsorption by nanoparticles (NPs) in a cheap and safe nanobiocomposite was increased several times (713%) due to the synchronization of the controlled synthesis of nanobiocomposite (α-Fe2O3NPs/lemon peel (LP)/Fe3O4NPs) in the final stages of its nanoparticles growth with the removal process of Brilliance Green, compared to that of the separate synthesis from the removal process. It was only performed during the simultaneous adsorption and photodegradation (SAP) because of the stabilization of its NPs by the small substances obtained from dye photodegradation, unlike alone adsorption (AA) with agglomeration of its NPs. It turned out that only in the case of simultaneous nanobiocomposite synthesis with dye removal process during SAP, the percentage of dye adsorption by nanoparticles of nanobiocomposite is higher than that of organic substances of its LP. A competitive process was happened between NPs and the organic substances of LP in nanobiocomposite including hydrolyzable tannin, cellulose and effective alcohols, in the absence of performance of pectin at pH = 6.0 and, with participation of only pectin at pH = 4.0, for adsorption with and without photodegradation of the dye which was studied by reaching the quantitative values and the mass balances.