High-k metal oxides are gradually replacing the traditional SiO2 dielectric layer in the new generation of electronic devices. In this paper, we report the production of five-element high entropy metal oxides (HEMOs) dielectric films by solution method and analyzed the role of each metal oxide in the system by characterizing the film properties. On this basis, we found optimal combination of (AlGaTiYZr)Ox with the best dielectric properties, exhibiting a low leakage current of 1.2 × 10−8 A/cm2 @1 MV/cm and a high dielectric constant, while the film’s visible transmittance is more than 90%. Based on the results of factor analysis, we increased the dielectric constant up to 52.74 by increasing the proportion of TiO2 in the HEMOs and maintained a large optical bandgap (>5 eV). We prepared thin film transistors (TFTs) based on an (AlGaTiYZr)Ox dielectric layer and an InGaZnOx (IGZO) active layer, and the devices exhibit a mobility of 18.2 cm2/Vs, a threshold voltage (Vth) of −0.203 V, and an subthreshold swing (SS) of 0.288 V/dec, along with a minimal hysteresis, which suggests a good prospect of applying HEMOs to TFTs. It can be seen that the HEMOs dielectric films prepared based on the solution method can combine the advantages of various high-k dielectrics to obtain better film properties. Moreover, HEMOs dielectric films have the advantages of simple processing, low-temperature preparation, and low cost, which are expected to be widely used as dielectric layers in new flexible, transparent, and high-performance electronic devices in the future.