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Ar+-ion-sputtered surface of KLN crystal was studied by X-ray photoelectron spectroscopy in order to investigate the oxidation states and chemical environments of K, Li, Nb and O ions. As Ar+-sputtering time increased, the decreasing binding energy of Nb 3d and the peak broadening of mixed Nb 4s and Li 1s (namely Nb* 4s) levels were observed. Also, the binding-energy di erence between O 1s and Nb* 4s increased as Ar+-ion-sputtering time increased. The broad peak of Nb* 4s was considered to be related to the site occupancy of Li ion in A1 and C in tetragonal tungsten-bronze structure.