Thiocyanate (SCN-) is used in many industrial processes and is found in industrial wastewaters. Adsorptive removal of thiocyanate by surfactant-modified coir pith, an unwanted byproduct of coir fibre industry was studied. Cationic surfactant, hexadecyltrimethylammonium bromide was used as modifier. Optimum pH for maximum adsorption of SCN- was found to be 2.0. Langmuir, Freundlich and Dubinin Radushkevich (D-R) isotherms were used to model the adsorption equilibrium data and the system followed all the three isotherms and the adsorption capacity of the adsorbent was found to be 8.6 mg g(-1). Kinetic studies show that the adsorption obeyed second order. Desorption studies showed that upto 90% recovery of SCN- from the spent adsorbent was feasible. Effect of foreign anions on the adsorption of SCN- was also examined.