expansion increases the bandwidth and reduces the density of states (DOS) of the Fermi level, however, the strong orbital hybridization between Ru 4d and O 2p of SRO will enhance the DOS, resulting in ferromagnetic interaction and metallicity, and the Curie temperature (T c ) of bulk SRO as high as 160 K. [16,17] SRO also has good electrical conductivity, thermal property, and chemical inertia, and has a high lattice matching degree on a variety of commonly used substrates. [18,19] Recent research on SRO heterostructures and superlattices with ultra-thin SRO layer further show remarkable phenomena. Typical examples include the ferroelectric tunable topological Hall effect (THE), [20][21][22][23][24] skyrmion in BaTiO 3 /SrRuO 3 , [9] and spin chirality fluctuation in 2D SRO ferromagnets with perpendicular magnetic anisotropy. [25] Besides, SRO is also used extensively in the study of anomalous Hall effect (AHE). [8,9,26,27] In SRO, both the AHE and THE of the SRO/STO heterostructure show a strong SRO thickness (t SRO ) dependence. If the thickness is not accurate or uniform, areas with different thicknesses will be superimposed, resulting in an artificial THE signal. [28] Therefore, a layer-by-layer growth mode is desired to precisely regulate the thickness at the unit cell (u.c.) level.However, quite different from many perovskite oxides such as La 2/3 Sr 1/3 MnO 3 , LaCoO 3 , and SrTiO 3 , where a layerby-layer growth mode can persist for even 100 unit cells, the SRO usually quickly transits from layer-by-layer mode into step-flow mode. According to previous studies, when SRO thin film is grown on a TiO 2 -terminated (001) STO substrate, the terminated atomic layer changes from the B-site to the A-site in the first period, [29,30] resulting in the transition from 2D layerby-layer mode to step-flow mode. In step-flow growth mode, the RHEED intensity does not oscillate and remains stable, making the thickness of the films impossible to be intuitively monitored by RHEED. Therefore, it is difficult to accurately control the thickness of superlattices and multilayer films.In this paper, we report the exploration of layer-by-layer growth of SRO. The epitaxial SRO thin films and (SRO n /STO 5 ) 10 superlattices were grown on TiO 2 -terminated (001) STO substrates. The single TiO 2 -terminated (001) STO substrates were obtained through standard buffered oxide etch (BOE) One of the keys to the construction of metal oxide heterostructures is the short characteristic length scale, which requires controlled growth and interface engineering on an atomic level. At present, the growth mode of SrRuO 3 (SRO) thin films grown on TiO 2 -terminated (001) SrTiO 3 (STO) substrates usually transitions from 2D layer-by-layer to step-flow at the first few growth periods, which is not conducive to the construction of superlattices or multilayer films. In this paper, persistent layer-by-layer growth of SRO thin films is demonstrated by regulating the growth conditions. As a result, the thickness can be precisely controlled down to a sing...