Theinsitucleaning of a substrate surface by low‐energy ion bombardment is discussed concentrating on the effect on the quality of sputter‐deposited metal thin films. The removal of carbon from the wafer surface with the addition of H2to Ar plasma atmosphere during theinsitucleaning was confirmed by secondary ion mass spectrometry evaluation. High crystallinity Ti films were obtained by deposition using Ar/H2insitucleaning by low‐energy ion bombardment. By the introduction of the Ar/H2plasmainsitusubstrate surface cleaning, Ti film growth by sputtering was confirmed to improve its crystallinity and its surface smoothness.