Previous studies have reported segregation of the minority element to the surface at both ends of the gold–nickel phase diagram. These results, which contradict the predictions of bond‐breaking arguments, were attributed to strain effects arising from the large atomic size difference between gold and nickel. Such effects for this and other alloy systems have been calculated by an elastic continuum model which suffers from several limitations. A pair‐potential model is proposed here which overcomes these difficulties. Dilute alloys of gold and nickel were studied by ion‐scattering spectroscopy to test these predictions. The calculations predict and the measurements show that the surface of either gold‐rich or nickel‐rich alloys becomes enriched in gold.