The use of laser annealing in the preparation of a clean, well‐ordered Ni(001) surface has been investigated. The surface was cleaned by argon ion bombardment and subsequently irradiated with the fundamental output of a high power, Q‐switched ruby laser. The laser treated surface was characterized by use of Auger electron spectroscopy and both conventional and spin‐polarized LEED, and the data compared to that from a surface prepared by thermal annealing. Laser irradiation of a sputtered surface at energy densities of ∼0.8 J cm−2leads to complete removal of residual argon without segregation of carbon or other contaminants at the surface. However, irradiation at an elevated temperature ∼200 °C is required to obtain a well‐ordered surface. At elevated temperatures, laser annealing provides a surface with cleanness and surface order comparable to that obtained by conventional thermal annealing.