CuInSe2surfaces can be cleaned by bombardment with Ar ions at glancing incidence and with energies up to 1.5 keV without change in composition. At near‐normal incidence a slight depletion of Cu is observed. The surface crystallinity can be partially restored by annealing to ∼550 °C, without preferential evaporation of an element. On Ar+‐cleaned and annealed surfaces, single‐crystal low‐energy electron diffraction patterns of CuInSe2have been produced for the first time.