The grain sizes and their influence on the roughness of an HfO2 single layer prepared with ion-assisted deposition were investigated. Three methods, x ray diffractometry, atomic force microscopy, and the k-correlated power spectral density function model, were used to obtain the grain sizes in two HfO2 single layers with 16 and 20 nm thicknesses. X ray diffractometry showed that the grain sizes were about 7 and 9 nm, respectively, whereas the other two methods demonstrated that the grain sizes were about 14 and 16 nm. It was thought that x ray diffractometry underestimated the grain size due to micro strain or a shallow penetration depth. The grains in an HfO2 single layer lead to a rough surface, which had a significant bulge at the middle-high frequency range in a power spectral density function curve. The coating intrinsic roughness of the HfO2 single layer was separated from the substrate roughness.