Selectivity coefficients for the competitive adsorption of chloride, bromide, and iodide at the air/solution interface have been measured by a high accuracy ion flotation technique using the surfactant cations dodecylammonium, dodecylmethylammonium, dodecyldimethylammonium, and dodecyltrimethylammonium. Selective binding was found to depend on the nature of the head group, with selectivity increasing from primary to quaternary ammonium ions, Results are consistent with counterion binding arising from contact adsorption by mutual dehydration of head groups and counterions.