Several models have been proposed to predict the direction and extent of surface segregation in binary metal alloys. Auger electron spectroscopy (AES) has proven useful to study these systems qualitatively, but the results of AES have proven difficult to quantify. Ion scattering spectroscopy (ISS) offers an alternative having true first‐monolayer sensitivity. ISS was used to study surface segregation in the Ag–Au and Pt–Cu systems. Results are compared with previous findings and model predictions.