The sorption abilities of thermally activated powders of leaves, stems and their ashes of Thespesia populnea and Pongamia pinnata plants have been probed for the extraction of Methyl Orange Dye from polluted waters. Various Physicochemical parameters such as pH, time of equilibration and sorbent dosage, have been optimized for the maximum removal of the Dye. The Dye sorption has been found to be sensitive to pH and high affinity of the sorbents towards the Dye has been found around pH: 3. Ashes have been found to be more effective than raw biomaterials. Fivefold excess of common trivalent and divalent anions ions present in natural waters, markedly affected the % of removal than monovalent ions. Cation like Ca2+, Mg2 , Cu2+ Fe2+ and Zn2+ have interfered to some extent. The methodologies developed have been applied to industrial effluents.