current, good stability, and large-area scalability. [6,7] In particular, AOSs that can replace the conventional polycrystalline Si have been actively researched in displays due to the growing demands for highresolution and high-frame-rate displays. [8] To obtain high-mobility AOSs, various multicomponent oxide systems have been investigated including In-Zn-Sn-O [9] (IZTO), In-Ga-Zn-O, [10] In-Ga-Sn-O, [11] and Al-In-Zn-O [12] channels. In the case of multicomponent AOSs, electrical properties such as field-effect mobility, threshold voltage (V TH ), and on/off ratio are strongly dependent on the cation ratio. Therefore, to find the optimal cation ratio, a combinatorial study on various cation components has been typically carried out. [13,14] However, although the conventional combinatorial approaches can allow successful discovery of optimal cation ratios, rather exhaustive experimental procedures are usually required, especially when there are many different cationic components to examine. Moreover, the complicated contributions from extrinsic parameters on thin-film transistor (TFT) mobility value, such as film quality and interface effects, make the determination of optimized device challenging, even with extensive first-principle study on amorphous multicomponent semiconductors using huge computation cost. [15,16] In this regard, machine learning (ML)-based synthetic approach can be a promising solution to optimize the cation ratio by predicting the electrical properties of multicomponent AOSs with a minimal trial and error via reduced number of experimental data.As is well known, ML is a technique that predicts the results by learning the patterns of training data. For this reason, ML has been widely utilized in various applications such as speech recognition, natural language processing, and robotics control. [17] Recently, using the ML, there has been a lot of interest in revealing the complex correlation between composition, processing, structure parameters, and electrical properties of various material systems. For instance, the discovery of new ternary oxide compounds for metallic glasses [18] and batteries, [19] and parameterizing the point defects in fin field-effect transistors [20] and band gap in inorganic solids [21] have been reported. In the case of multicomponent AOSs, although the ML can be aThe ORCID identification number(s) for the author(s) of this article can be found under https://doi.org/10.1002/smtd.202101293.