Arsenic and fluoride are recognized globally as the most serious inorganic contaminants in drinking water. As there is no safe and effective treatment for the cases of fluoride poisoning and combined arsenic-fluoride toxicity, the present study was planned to assess (i) the mechanism of combined exposure to arsenic and fluoride via biochemical and spectroscopic data; (ii) the effect of a thiol chelating agent, meso-2,3-dimercaptosuccinic acid (DMSA), either individually or in combination with the antioxidant vitamin C in reversing arsenic-fluoride toxicity; and (iii) whether combination therapy enhances arsenic and fluoride removal from blood and soft tissues.