This study aims to evaluate the functionalization of chitosan biopolymer with heterocyclic moieties of 2-thioxodihydropyrimidine-4,6(1H,5H)-dione used for enhancing the sorption of Cr ions from aqueous solution. A synthesized sorbent is a nanoscale particle (around 5–7 nm), which explains the fast kinetics of sorption. The sorbent is specified using elemental analysis (EA), FTIR, BET (nitrogen sorption desorption isotherms), TGA, and SEM-EDX analyses. Sorption properties are investigated using ultraviolet emission (UV) but also using visible light (L). In the sorption diagram, the high sorption uptake and fast kinetics observed using ultraviolet conditions are shown. This work is conducted by removing Cr ions from highly contaminated tannery effluents, which have a high concentration of Cr associated with other poisonous elements such as Cd(II) and Pb(II). Under the selected conditions, complete sorption is performed during the first 60 and 45 min with a capacity of 2.05 and 2.5 mmol Cr g−1 for the crosslinked chitosan (without functionalization) in L and UV, respectively. This sorption is enhanced by functionalizing to 5.7 and 6.8 mmol Cr g−1 at the L and UV, respectively, as well as improving the sorption kinetics to 35 and 30 min for both techniques, respectively. The PFORE, and (Langmuir and Sips equations) fit the kinetics and isotherms, respectively.