Materials informatics exploiting machine learning techniques, e.g., Bayesian optimization (BO), has the potential to offer high-throughput optimization of thin-film growth conditions through incremental updates of machine learning models in accordance with newly measured data. Here, we demonstrated BO-based molecular beam epitaxy (MBE) of SrRuO3, one of the most-intensively studied materials in the research field of oxide electronics, mainly owing to its unique nature as a ferromagnetic metal. To simplify the intricate search space of entangled growth conditions, we ran the BO for a single condition while keeping the other conditions fixed. As a result, high-crystallinequality SrRuO3 film exhibiting a high residual resistivity ratio (RRR) of over 50 as well as strong perpendicular magnetic anisotropy was developed in only 24 MBE growth runs in which the Ru flux rate, growth temperature, and O3-nozzle-to-substrate distance were optimized. Our BO-based search method provides an efficient experimental design that is not as dependent on the experience and skills of individual researchers, and it reduces experimental time and cost, which will accelerate materials research. The itinerant ferromagnetic perovskite SrRuO3 is one of the most promising materials for oxide electronics. 1 -10 Owing to its compatibility with other perovskitestructured oxides, as well as its high conductivity and chemical stability, 3 SrRuO3 is widely used as an epitaxial conducting layer in oxide heterostructures. However, a thorough understanding of its transport properties, electronic structure, and origin of its ferromagnetism remains elusive despite tremendous efforts for over five decades. While high-quality specimens are indispensable for exploring electronic states, it is difficult to make high-quality bulk single crystals of SrRuO3, and hence, thin film specimens have been making a significant contribution to such research. The residual resistivity ratio (RRR), which is defined as the ratio of resistivity at 300 K [ρ(300 K)] to that at 4 K [ρ(4 K)], is a good measure of the purity of a metallic system, and accordingly, the quality of single-crystalline SrRuO3 thin films: RRR is very sensitive to defects and offstoichiometry. 8,11,12 More specifically, only SrRuO3 films with high RRR values above 40 and 60 have enabled observation of sharp dispersive quasiparticle peaks near the Fermi level by angle-resolved photoemission spectroscopy (ARPES) and of quantum oscillations in the electrical resistivity, respectively. 13,14 Such high-quality films maintain their metallic and ferromagnetic character even when the thickness is reduced to a monolayer, 15 providing a rare example of two-dimensional ferromagnetism. This means that extremely thin SrRuO3 films can serve as a two-dimensional spin-polarized electron system, as the existence of a spin-polarized electron current has been established in thicker SrRuO3-based magnetic tunnel junctions. 16,17 Accordingly, high-quality SrRuO3 thin films are also promising for future spintronics application...