The novel, single-sample concept combinatorial method, the so-called micro-combinatory technique, has been shown to be suitable for the high-throughput and complex characterization of multicomponent thin films over an entire composition range. This review focuses on recent results regarding the characteristics of different binary and ternary films prepared by direct current (DC) and radiofrequency (RF) sputtering using the micro-combinatorial technique. In addition to the 3 mm diameter TEM grid used for microstructural analysis, by scaling up the substrate size to 10 × 25 mm, this novel approach has allowed for a comprehensive study of the properties of the materials as a function of their composition, which has been determined via transmission electron microscopy (TEM), scanning electron microscopy (SEM), Rutherford backscattering spectrometry (RBS), X-ray diffraction analysis (XRD), atomic force microscopy (AFM), spectroscopic ellipsometry, and nanoindentation studies. Thanks to the micro-combinatory technique, the characterization of multicomponent layers can be studied in greater detail and efficiency than before, which is beneficial for both research and practical applications. In addition to new scientific advances, we will briefly explore the potential for innovation with respect to this new high-throughput concept, including the creation of two- and three-component thin film databases.