The sludge, which was collected from a biological coke wastewater treatment plant, was used as a low-cost adsorbent in the removal of reactive dyes (Methylene Blue (MB) and Reactive Red 4 (RR4)) from aqueous solution. The pH of dye solution played an important role on the dye uptake. With the solution pH increase, the MB uptake increased; whereas the RR4 uptake decreased. The maximum uptake of RR4 by protonated sludge was 73.7 mg/g at pH 1, and the maximum uptake of MB by sludge was 235.3 mg/g at pH 9. Three functional groups, including carboxyl, phosphonate, and amine group, were identified by potentiometric titration, fourier transform infrared (FT-IR) spectrometry, and X-ray photoelectron spectroscopy (XPS). The anionic functional groups, phosphonate and carboxyl group, were identified as the binding sites for the cationic MB. Amine groups were identified to bind RR4. The main mechanism of the reactive dyestuffs adsorption is electrostatic interaction.